May198£
Do not remove. This document
EPA-450-4-88-007 should be retained in the EPA
Region 5 Library Collection.
Statistical Properties Of Hourly
Concentrations Of Volatile Organic
Compounds At Baton Rouge, Louisiana
By:
Alison K. Pollack
Thomas J. Permutt
Mithra Moezzi
Systems Applications, Inc.
San Rafael, CA 94903
Contract No. 68-02-4331
EPA Project Officers: William F. Hunt, Jr.
Robert B. Faoro
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office of Air and Radiation
Office of Air Quality Planning and Standards
Research Triangle Park, North Carolina 27711
U.S. ion Agency
12ft Floor
Chicago, IL 60604-3590
-------
This report has been reviewed by the Office of Air Quality Planning And Standards, U S Environmental
Protection Agency and approved for publication as receivec from the contractor Approval aoes net signify
tnat the contents necessarily reflect the views and policies of the Agency, neither does mention of trade
names or cortimercial products constitute endorsement or recommendation for use
EPA-450/4-88-007
-------
Contents
Acknowledgements i
Excutive Summary ii
1 INTRODUCTION 1
2 MONITORING SITE AND DATA BASE DESCRIPTION 2
3 DISTRIBUTIONS OF HOURLY CONCENTRATIONS 5
4 RELATIONSHIPS BETWEEN MEAN AND PEAK CONCENTRATIONS 10
5 ANALYSIS OF VARIANCE MODELS 19
6 CONCLUSIONS 27
References 28
Appendix A: Summary Statistics and Lognormal Probability Plots
Appendix B: Scatterplots of Daily Peak 1-Hour, 3-Hour, and
8-Hour Average Versus Daily Mean Concentrations
Appendix C: Analysis of Variance Tables and Least Squares Means
8715^1 1
-------
Acknowledgements
The authors would like to thank Gustave von Bodungen and Jim Haziett of the Loui-
siana Department of Environmental Quality for making available the data discussed
in this report, for providing information on the monitoring site and methods, and for
valuable assistance in data interpretation. We also acknowledge the assistance of
Bob Johnson, our in-house computer expert, for transporting the data from the
Louisiana DEQ computers.
87lS»+rl
-------
EXECUTIVE SUMMARY
Hourly measurements of 16 volatile organic compounds (VOC) in downtown Baton
Rouge, Louisiana have been monitored since 1984. These are probably the most
extensive data of hourly air toxics concentrations in the United States collected to
date. In this report we discuss the results of an exploratory data analysis of nearly
two years of hourly concentrations. Although we analyzed the data for all VOCs
monitored, and present our conclusions for all data, our discussion centers on
benzene, a known human carcinogen.
The hourly concentration distributions are extremely heavy-tailed; most of the
concentrations are low, but there are a fair number of very high concentrations.
Most of the pollutants are well characterized by a lognormal distribution.
The data set provides a unique opportunity to see how well daily maximum one-hour
concentrations can-be predicted by 24-hour averages. At lower concentrations there
is a strong correlation between the maximum hourly average and the 24-hour mean.
At higher concentrations, however, the relationship is much weaker. Twenty-four
hour means can indicate days on which very high hourly concentrations occur, but
cannot reliably predict the magnitude of these peaks. Daily maximum three-hour
and eight-hour averages are more highly correlated with 24-hour means, and can
therefore be predicted more reliably by 24-hour means.
Analysis of variance models were fitted to the data to see if the variability in the
concentrations can be explained by wind direction, hour of the day, day of the week,
and month. All four variables were found to be statistically significant, but explain
only a small percentage of the total variability in the measurements. From the
analysis of variance modeling, concentration averages by hour, wind direction, day,
and month were calculated; the averages for benzene were plotted. Benzene
concentrations peak during morning and evening rush hours, are low on weekends
(especially Sundays), and are highest in January. Most interesting are the patterns by
wind direction. Benezene concentrations are highest when the winds are from the
north, presumably attributable to a large chemical industrial complex north of Baton
Rouge. The results of the analysis of variance for all VOCs are similar to tnose for
benzene.
87 1
-------
1 INTRODUCTION
The Louisiana Department of Environmental Quality has measured concentrations of
16 species of volatile organic compounds hourly at the state capital in Baton Rouge
since 1984. These are probably the only such extensive data on .hourly concentrations
of volatile organic compounds in the United States. The aata ser provides an oppor-
tunity for interesting analyses of ambient volatile organic compounds concentra-
tions. In this report we present the results of an exploratory data analysis.
Our analysis of these data is focused largely on the possibilities for making
inferences about hourly concentrations from more limited data. In Section 2 we
describe the monitoring methods and discuss the major emission sources that influ-
ence the site. In Section 3 we examine the distribution of the hourly measurements,
giving particular attention to the higher concentrations. In Section 3 we discuss the
extent to which peak short-term concentrations can be predicted from 24-hour
average concentrations. In Section 4 we consider how well hourly data can be pre-
dicted on the basis of seasonal, diurnal, and meteorological patterns. We conclude by
discussing potential future analyses of this unique data set.
8 7 1 5^r 1 2
-------
2 MONITORING SITE AND DATA BASE DESCRIPTION
Since 1984 the Louisiana Department of Environmental Quality has been collecting
hourly measurements of volatile organic compounds (VOC) in downtown Baton Rouge
near the state capitol. The monitor is based in an office building and collects
ground-level measurements. Several major sources of emissions are within a few
miles of the monitoring site. A major state highway circles the downtown area about
a mile to the south and east. There are fuel transfer operations on Mississippi River
barges to the northwest. Most important, there is a large industrial complex due
north of the site, stretching from about one and one-half mile away to about three
miles away. Located in this complex are two oil refineries and five chemical plants.
Sixteen volatile organic compounds are measured hourly by dual computer controlled
gas chromatographs. Eight hydrocarbon species are measured by a flame ionization
detector (FID). They are benzene, toluene, ethyl benzene, m-xylene, propane,
butane, hexane, and pentane. In addition, unknown and total hydrocarbons are mea-
sured. Eight chlorinated hydrocarbon species are measured by a Hall electrolytic
conductivity detector (HECD). They are vinyl chloride, methylene chloride, 1,1-
dichloroethane, chloroform, ethylene, dichloride, carbon tetrachloride, trichloro-
ethylene, and perchloroethylene. Unknown chlorinated hydrocarbons and total
chlorinated hydrocarbons are also determined. Meteorological parameters collected
hourly are wind speed, wind direction, and ambient temperature.
Although the concentrations are reported as hourly averages, the actual period of
continuous air intake sample collection is 20 mintues for the FID and 25 minutes for
the HECD. The remaining portion of the hour is required for gas chromatograph
sample analysis. The instrumentation is automatically calibrated every day between
1100 and 1400, so only 21 hourly samples per day are actually collected. The mea-
surement system and the quality assurance features are described in detail.elsewhere
(LADEQ, 1986).
Although the monitoring site has been in operation since 1984, construction near the
monitoring site until September 1985 was thought to result in anomalous and
unreliable measurements; we therefore excluded these observations. In this analysis
we examined over 11,000 hourly measurements taken between 3 October 1985 and 30
June 1987.
87 1
-------
Figure 2-1 shows the relative abundance of each of the hydrocarbon species mea-
sured, based on average hourly ppbv concentrations. The largest proportion, 33 per-
cent, comprises unknown hydrocarbons. Of the identifiable hydrocarbons, propane
and butane each account for 18 percent of the total. Next in abundance are toluene
and benzene, which account for 13 and 10 percent, respectively, of total hydrocar-
bons. In this report we concentrate mainly on the hourly concentrations of benzene,
a known human carcinogen.
87 1 5>*r 1 2
-------
Propane
Unknown
hydrocarbons
M-xylene
Ethyl benzene
Toluene
Butane
FIGURE 2-1. Hydrocarbon composition by species
(based on average hourly ppbv concentrations).
-------
3 DISTRIBUTIONS OF HOURLY CONCENTRATIONS
The most basic and one of the most useful ways to analyze the approximately 11,000
hourly measurements of each species is to try to describe the statistical distributions
of the concentrations. This will provide direct answers to such questions as, "How
often is the hourly concentration of benzene above 10 ppbv?" Furthermore, a sta-
tistical characterization of these concentration distributions might be useful in mak-
ing inferences about hourly concentrations at a site where concentrations are not
measured hourly.
The distribution of benzene concentrations is fairly typical. A cumulative frequency
distribution for benzene concentrations below 10 ppbv is presented in Figure 3-1 and
summary statistics are listed below in Table 3-1.
TABLE 3-1. Summary statistics for benzene.
No. of hourly observations = 11,306
Mean = 5.76 ppbv
Standard deviation = 20.20 ppbv
Minimum = 0.0 ppbv (21%)
Percentiles (ppbv):
25th percentile = 0.6
50th percentile = 1.8
75th percentile = 4.1
90th percentile = 10.3
95th percentile = 20.2
99th percentile = 82.89
Highest observations (ppbv):
708 Jan. 25, 1986
494 Mar. 4, 1986
462 Mar. 6, 1986
408 Jan. 13, 1986
378 Jan. 13, 1986
87 1 5*r1 2
-------
100.0%
o
c
0)
cr
03
03
JS
3
E
3
O
01 23456789 10
Benzene, ppbv
FIGURE 3-1. Cumulative frequency distribution of benzene
concentrations less than 10 ppbv.
-------
Over 20 percent of the measurements are zero: in a large orooortion of the hours r.o
benzene was detected at all. Many more measurements are not much above zero:
the lower quartile is 0.6 ppbv, the median is 1.8 ppbv, and 90 percent of the mea-
surements are less than 10.3. The highest measurements are very far from zero
indeed: the maximum is 708 ppbv, four measurements are over 500 ppbv, and about
100 are over 100 ppbv. The five highest values all occur in January or March, and
two of the five highest values are on the same January day in 1986. A cause for
unusually high concentrations is sought by LADEQ staff when they occur. In most
cases, the highest concentrations are associated with an unexpected release from one
of the nearby chemical facilities.
The summary statistics in Table 3-1 indicate that the distribution of benzene concen-
trations is characterized by low levels for the majority of the hours but very high
levels for a small proportion of the hours. Such a heavy-tailed distribution is com-
mon for hourly pollutant measurements, which can often be well described by a log-
normal distribution (Ott, 1986). Figure 3-2 is a lognormal probability plot of the
concentrations of benzene. The vertical axis is the van der Waerden normal score, or
the value from the standard normal distribution that would be expected to have a
given rank. For example, the 84th percentile is assigned a normal score of one
because one standard deviation above the mean of a normal distribution is the 84th
percentile. The horizontal axis is the common logarithm of the concentration.
Values of zero were assigned a logarithm of -1.5. If the points in a lognormai proba-
bility plot fall along a straight line, we can conclude that the measurements do
indeed arise from a lognormal distribution.
In viewing Figure 3-2 it should be kept in mind that the single point at abcissa -1.5
represents about 20 percent of the data, and the other Z's in the lower portion of the
curve also represent many observations each. The figure therefore shows mainly the
upper tail of the distribution.
The points are in a fairly straight line over a considerable range, from benzene con-
centrations of less than 1 ppbv (log 1 = 0) to the maximum concentration of 708 ppbv
(log 708 = 2.85). Thus the lognormal distribution is a fairly good fit to the empirical
distribution in this range. The bending of the curve at concentrations below 1 ppbv is
perhaps not too important. Although there are a great many concentrations in this
range, they are only reported to one significant figure, and may be close to the limit
of detection. If the measurements were reported to two or three significant digits
(as the higher concentrations are), then the bending of the curve at concentrations
below 1 ppbv might not occur.
This distributional fit offers the possibility of getting at Least a rough idea of tne
behavior of the extreme hourly concentrations from less extensive data. Suppose
that only a few hundred hourly concentrations were available to estimate the 90th
and 95th percentiles. This would be sufficient to estimate the 90th and 95th percen-
tiles fairly accurately. Assuming the logarithms of the concentrations are normal
87 IS^r 1 2
-------
CRIK
22 !
V22D
222
2221
L i 1 1
222
222
222
22
22
22
2
22
22
2:2
222
22
2
2 2 2
2222
». "t Sbu> 06i
or o i
loglO 6rfU ere
FiGUHE 3-2. Lognonrai probability plot of hourly benzene concentrations.
("A" = one observation, "B" = two observations; etc.; "Z" = 26 or more
observations.)
-------
with mean u and 'standard deviation ^, the following simultaneous equations could be
solved for u and c:
u •*• 1.2&o = log PQQ and
u + 1.65c = log
This amounts to fitting a straight line through the 90th and 95th percentiles on the
probability plot. The estimated values of y and a could then be used to estimate
fairly extreme quantiles. For example, the characteristic monthly maximum, the
value that is exceeded one hour per month in the long run, can be estimated by the
upper 1/720 quantile of the fitted lognormal distribution. For a standard normal dis-
tribution, the 1/720 upper quantile is 2.9S. The characteristic monthly maximum
could be estimated by the antilogarithm of u + 2.98o after u and a have been esti-
mated.
As a numerical example, consider benzene. As shown in Table 3-1, the observed 90th
and 95th percentiles are 10.3 and 20.2 ppbv. This gives u = 0.00 and a = 0.79. The
characteristic monthly maximum would therefore be estimated as log" [0.00 +
(2.98-0.79)] = 227 ppbv. In fact, the observed upper 1/720 quantile is 234. The esti-
mated characteristic monthly maximum is very close indeed to that predicted by this
simple logarithmic fit to the data. This is not the case for all of the VOCs. For
example, the actual characteristic monthly maximum for butane, 352,. is a factor of
two larger than the estimate of 186. This gives a fair picture of the limitations of
the technique. Obviously this method of estimation is not accurate enough to
determine compliance with a standard. However, for a distribution spanning a range
of concentrations from zero to hundreds of times the median, the method may pro-
vide a rough estimate of the magnitude of extreme events not otherwise available.
Summary statistics and lognormal probability plots for the other species are in
Appendix A. The results are substantially similar to those for benzene.
87 1 5"+r 1 2
-------
RELATIONSHIPS BETWEEN MEAN AND PEAK CONCENTRATIONS
The relationships between the 24-hour mean and daily maximum one-hour, three-
hour, and eight-hour average concentrations were investigated in order to assess how
well measurements of 24-hour concentrations can represent daily short-term peaks.
The short-term maxima were computed using fixed block averaging; for example,
eight-hour concentrations were averaged for midnight to 0700, 0800 to 1500, and
1600 to 2300.
Correlation coefficients between daily average concentrations and the daily maxi-
mum one-hour, three-hour, and eight-hour average concentrations for each species
studied are listed in Table 4-1. The correlations between daily average and peak
one-hour concentrations range from a low of 0.53 for trichloroethylene to a high of
0.97 for carbon tetrachloride; most correlations are between 0.70 and 0.90. For
benzene, the correlation between daily average and peak one-hour concentrations
(based on 582 pairs of available data) is 0.85. Thus, 100(0.85) = 72 percent of the
variance about the mean of peak one-hour concentrations can be explained by the 24-
hour average concentration.
The correlation coefficient of 0.85 for benzene is considerably higher than the 0.65
determined in an earlier analysis of the Louisiana data (Permutt and Edland, 1987).
The earlier study used data between January 1985 and mid-July 1986, while the study
reported here uses data between October 1985 and June 1987. As noted above,
observations before October 1985 are believed to be anomalous; their inclusion in the
earlier study and exclusion from the current study may account for the noted dis-
crepancy in correlation coefficients.
As one would expect, correlations generally increase as averaging periods for the
peak increases. Correlations between 24-hour average and peak eight-hour concen-
trations are above 0.90 for most species. In general, correlations between 24-hour
mean and peak 1-, 3-, and 8-hour concentrations for the hydrocarbons are higher than
those for the volatile organic compounds.
Scatterplots of daily mean benzene concentrations against peak 1-hour, 3-hour, and
8-hour concentrations are shown in Figure 4-1. In all of the plots a line with slope
equal to the number of short-term averaging periods in one day's data forms a
natural upper bound for the ratio of the peak short-term concentration to daily mean
concentration. A full set of plots for all species is included in Appendix B.
10
-------
TABLE 4-1. Correlations of daily mean and peak 1-, 3-,
and 8-hour concentrations.
Compound
n-Propane
n-Butane
n-Pentane
n-Hexane
Benzene
Toluene
Ethyl Benzene
m-Xylene
Unknown HC
Total HC
Vinyl Chloride
Methylene Chloride
Dichloroethylene
Chloroform
Ethylene Bichloride
Carbon Tetrachloride
Trichloroethylene
Perchloroethylene
Unknown VOC
Total VOC
1 Hour
0.65
0.88
0.86
0.78
0.85
0.88
0.90
0.82
0.83
0.81
0.84
0.83
0.74
0.67
0.85
0.97
0.53
0.82
0.71
0.72
3 Hours
0.80
0.93
0.92
0.86
0.88 '
0.92
0.93
0.88
0.89
0.89
0.86
0.80
0.63
0.65
0.84
0.94
0.55
0.76
0.76
0.68
8 Hours
0.94
0.97
0.97
0.94
0.96
0.97
0.97
0.94
0.95
0.95
0.94
0.90
0.85
0.93
0.91
0.97
0.87
0.86
0.38
0.38
11
17 l 5»tr 3
-------
A '00
V
C
A
A
A
I
i A A AA A
!00 - A AA AA
I A AAAA A AA
I AA AA A6 A A
I CBCB6AAEA BAAACA 6
1 AT;zii.ECCCBBA»A
0 -Z222VC
0 5 10 15 20 25 30 35 40 45 50 55 60 65 70 '5 80 85 9P 95 lud iC'5 : 1I "j
*'.'> ?50 08S n!DCt»
FIGUPE 4-la. Daily mean benzene concentrations (ppbv) versus daily peak
one-hour concentrations. ("A" = one observation; "B" = two observations;
etc.; "Z" = 26 or more observations.)
12
-------
A
A
A A
A A A
A A A AA A
A AA A A A
AA A A BA BA
AAAABCCACAAA3A
FM>-E»Bfe A AA
0 S 10 15 20 25 30 35 40 «5 50 55 60 65 70 75 8u 65 9C 95 100 105 . . C '. : 5
aaily average oen:ene
MO'C J5C DBS MlDO[N
FIGUPE 4-Ib. Daily mean benzene concentrations (ppbv) versus daily
peak three-hour concentrations.
-------
100
A
A A
A
A
AA
A
A
A
1C - A
A A
A A A A A
' A A A A
A AA A A
,'j - A A 3 AAA5AAA
[ AAAA CA6A
ACBAEBAAC
AfLkiSB
5 10 15 ?0 ?5 30 35 40 OS SO 55 60 65 70 75 80 85 90 95 100 105 111 1!
flat)> average oerwene
?8 oes HIOOEK
FIGURE 4-lc. Daily mean benzene concentrations (ppbv) versus daily
peak eight-hour concentrations.
-------
The peak short-term benzene concentrations show considerable scatter ir the 'jpper
fifth percentile of daily means. In the lower range of the data the linear reiauonsnip
between daily mean and peak shori-term concentrations is relatively strong. Plots
for many of the other species exhibit similar patterns. As can be seen from the
plots, linear regression predictions of peak concentrations based on the daily mean
concentrations would substantially overpredict or underpredict many of the observed
values in the high concentration range. In particular, the two highest observed one-
hour concentrations, 708 ppbv and 494 ppbv, would be grossly underestimated.
In general, the peak three- and eight-hour benzene concentrations show less scatter
than the one-hour concentrations, as would be expected. Regression predictions of
the two highest observed three-hour concentrations would be substantially under-
estimated. Regression predictions of the highest eight-hour benzene concentrations
would be fairly close to the observed values.
The extreme points may strongly influence the correlation coefficient, since they
contribute heavily to the covariance between the daily mean and peak short-term
concentrations. Since, as we observed in the previous section, the distributions of
hourly concentrations are very heavy-tailed and fit reasonably well to a lognormal
distribution, a logarithmic transformation of the short-term maxima will reduce the
influence of the extreme observations on the correlation and hence the regression.
Scatterplots of logarithmic daily mean benzene concentrations against logarithmic
daily peak 1-hour, 3-hour, and 8-hour concentrations are shown in Figure 4-2. All
three scatterplots show much stronger correlations than the untransformed data.
Regression predictions would still underestimate the highest one- and three-hour
daily maxima, but not as substantially as the regressions based on the untransformed
averages.
In summary, correlation coefficients between daily mean and short-term maximum
concentrations are high; but if a regression line were drawn, the peak concentrations
in the upper ranges of concentration would be highly scattered about the line. Due
to this variability, a linear regression model may often not provide accurate predic-
tions of the highest one-hour concentrations from 24-hour concentrations. Taking
logarithms of the short-term averages strengthens the correlations and improves the
accuracy of the regression predictions, but still may not provide accurate enough
predictions of peak short-term concentrations.
87 1 5-*r 1 2 15
-------
1.5
1.0
0.5
0.0
-0.5
-1 .0
-1.5
AA
*
AA A
A A
A A A AC
AA AAIAAAAB
A A I CA AA AAAAI A
AA A CAO IAC A AAA A
AIA IAA AAC18 A A
»A A
BAA
II A B
A AA
• AA CBAICAfAJ
A AA tOAAIAffd 08
A A AAKOAADOf IFOCA
A I IAAAAIC ClABASIFCOOOCA A
t AA8« AA ACAKFFllll JAI C
I A JA A88 ACffHCrjOtOJJA A
A A CACDAUCBCMCDCB6A A
A A A AAA AFOC CCBCBAA
C A A8 Af AABABA B
AA iAAAA t
A AA A A A A A
A A A
A
A
A
-1.5
-0.5
0.0
0.5
L5SM.'»(>1
FIGURE 4-2a. Log daily mean benzene concentrations (ppbv) versus daily
peak one-hour concentrations. ("A" = one observation; "3" = two
observations; etc.; "Z" = 26 or more observations.)
16
-------
LGBN2NC i
J.5
2.0
1.5
1.0
0.5
0.0
-0.5
-1.0
-15 - M
-2.0
AAA
AA
A A
ABA
A
A AA A
B
B A AA 8
AA A AA
A
AA
A AAA8B
AA AA BA A
A A A A A C
AA A AB BABAA8A
A C AAB A AB BA
AB CAACA A A A
BBO AO CBCB A A
A AA 3EOBBCC A
A A BBACCOCHGCDB A A
BC CEEAC8JECBB C
AA A B 8AC8ADEDEFCEJBOCABA
AA AOABBB8COIEUGGHCCAA
A CADACCCCEIDEEA A
AAC CAOCAC8CDFA
BCAAECAC8CAA
AC AAB8 AA
1A AA
AA
AA
A
-1.0
-0.5
0.0
0.5
LGBNZKFN
! .0
1 5
FIGURE 4-2b. Log daily mean benzene concentrations (ppbv) versus daily
oeak three-hour concentrations.
-------
2.0
A
AAAA
1.0
0.5
0.0
*
AA
6 A A A
A A AAAA
A A A
A
BBAAA
AAA A
SBO ABDA A
AA CACDBB AA
A BCDCBOA C
A ACEGOEE80
A A ABCACOFCGECAB
A AAAOFMOGGHOC
A AA CDHGrlOHFD
A A AAEBG1G1ICDB
CCB3BEBFEKIOB
A A CECGBOCDO
A A BCCCD 3 B
A AC08A8D A
A BA CAA A
C A AAA
AB
AA A A A
AAA C8A
BAA A
A A
AAA
A AA 8
AAAA
86AA
A
A
AA
-1.0
-0.5
0.5
L3BNZNEM
1.5
FIGURE 4-2c. Log daily mean benzene concentrations (pphv) versus daily
peak eight-hour concentrations.
18
-------
5 ANALYSIS-OF-YARIANCE MODELS
In an earlier analysis of the Louisiana data, concentrations of toxic gases averaged
for each combination of hour and wind direction were examined; a two-way analysis-
of-variance model was fit to describe the variation of concentrations with hour of
the day and wind direction (Permutt et al., 1987). Availability of tne full hourly data
set now allows several related issues to be investigated. First, some extra explana-
tory variables can be added to the model, e.g., the effects of season and day of the
week. Second, it is possible to transform the data; in view of the extreme skewness
and reasonable lognormal fit, a logarithmic transformation might be aesirabie.
Finally, and perhaps most important, it is possible not only to estimate the para-
meters of the best-fitting model but also to judge how well the model fits the
individual hourly measurements.
We fit a four-way anaiysis-of-variance model to the hourly concentrations of each of
the 20 species using SAS PROC GLM. The four classification variables were hour of
the day, wind direction, day of the week, and month. The hours range from zero
(0000 to 0100) to 23 (2300-2400); three midday hours are usually missing because of
instrument calibration and some data are erroneously identified as "hour 81". Wind
direction was converted from degrees into 16 compass points. A direction of 0
degrees (due north or DN) was treated as a separate category because calm winds
were sometimes recorded as direction 0, and this is different from north winds.
There is also an error category (ERR) for a few data with direction above 360
degrees. The days of the week are represented as 1 to 7, starting from Sunday, and
seasonal effects are represented by calendar month. We thus have a linear model
with 25+ 18 + 7 + 12 = 62 parameters, which are estimated simultaneously by linear
least squares. Because the design is unbalanced (e.g., there are more east winds in
some hours than others) the parameter estimates are not simple averages. The
average concentration for a given hour (or wind direction, day of the week, month),
controlling for the effects of the other variables, is estimated by the "least-squares
mean" for that hour (or other variable).
Table 5-1 is the analysis-of-variance table for benzene. Each of the four main
effects is significant at the 0.01 level, indicating that benzene concentrations cer-
tainly differ among hours, days, seasons and wind directions. Perhaps most remark-
able is the R value of 0.09. These effects, though highly significant, account for
only a small fraction of the variablity in benzene concentrations. We are therefore
left with enormous variation in hourly concentrations that cannot be explained by
seasonal, diurnal, weekly or meteorological effects and appears to be random.
Considering the extent of the range of concentrations, the skewness of the distribu-
tion over this range, and the reasonable lognormai fit to the distribution, it seems
87 15>*r 1 2 19
-------
000 =
•5
-P
4J
•H
U-4
M-J
o
4-H
CD
0
•H
-------
reasonable to try fitting the logarithms of the concentrations, rather than the con-
centrations themselves, as functions of the same four sets of explanatory variables.
This is equivalent to assuming a multiplicative rather than additive relationship ,
betweeen the effects of wind speed and hour, for example. The zero concentrations
present a problem in taking logarithms, of course; we somewhat arbitrarily took the
logarithm of 0 to be -1.5.
Table 5-2 is the analysis-of-variance table for log benzene. The R value is 0.1S, as
compared with 0.09 for the untransformed benzene concentrations. This logarithmic
fit may therefore be a slightly better way to describe the seasonal, diurnal, and
meteorological patterns of concentrations, but most of the variation in the concen-
trations still remains unexplained.
The least squares means for benzene are plotted by hour, wind direction, month, and
day in Figures 5-1 through 5-4, respectively. These plots show the least squares
means resulting from fitting the model to both the transformed and untransformed
data. The least squares means from the transformed data were back-transformed to
the original units and are thus geometric means. The geometric means are always
lower than the arithmetic means because they are much less influenced by the higher
concentrations.
Concentrations tend to be highest in the morning peak traffic period, as shown by the
relatively high least-squares means for hours 6 and 7 in Figure 5-1. Concentrations
are also relatively high during hours 20 and 21 just past the evening rush hour. It is
interesting to note that in the hour immediately after the midday calibration period
concentrations are higher relative to the following few hours. This may indicate
higher concentrations during the missing midday hours, when presumably traffic
increases.
Northerly winds are generally associated with relatively high benzene concentra-
tions. North of Baton Rouge is a large complex of refineries and chemical plants.
Concentrations tend to be relatively high in January (three of the five highest
recorded benzene concentrations occurred in January). Sundays have relatively low
concentrations, as would be expected.
It should be emphasized again that these effects, while highly significant, account
for very little of the variation in benzene concentrations. For example, the highest
hourly least-squares mean is 9.9 ppbv, and the lowest is 3.6 ppbv. This would appear
to be a significant difference, practically as well as statistically. Nevertheless, it
does not go far toward explaining concentrations as high as 500 ppbv.
The analysis-of-variance tables and least squares means for all species are in Appen-
dix C. The results are generally similar to those for benzene.
21
87 :
-------
0000
a
en
0
£5
4-1 C
C Q
sSI
£ >i
n
S-l -H
0 4-1
4-1 O
CD
33
en T3
B ^
re re!
0 4-1
O
en
a
fO H
4J
4-1
a
$
CO
o
o en 03 ci
— T — O
o a o\ —
O
O
o o o o
o o o o
0000
o o o o
o- o oo
I M
CSi —
o
CO
CSl ^-
O CTi
O
X
CO GO
o o
o en o as
22
-------
12
10 -
8 -
.a
o.
a.
g 6
N
O
CQ
4 -
Arithmetic mean
Geometric mean
0 2 4 6 8 1012141618202224
Beginning hour
FIGURE 5-1. Estimated mean benzene concentrations (ppbv) by hour.
23
-------
10
a
o
c
03
i • r ' i ' r T r ~~"i ' I T i • r ' I • T ' I • I • i—• I • i ' 1—' I
DN N NNE NE ENE E ESE SE SSE S SSW SW WSW W WNW NW NNW N
Wind Direction
FIGURE 5-2. Estimated mean benzene concentrations (ppbv) by wind direction.
24
-------
24-
22-
20-
18-
16-
.0
o
c
QJ
N
C
CD
CD
10-
8-
6-
4-
2-
Arithmetic mean
Geometric mean
Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec
Month
FIGURE 5-3. Estimated mean benzene concentration (ppbv) by month.
25
-------
8
7-
.a
a.
a.
c
CD
N
C
CD
CD
5-
4-
3-
2-
1 -
0
Mon Tues Wed Thurs Fri Sat Sun
Day of Week
FIGURE 5-4. Estimated mean benzene concentrations (ppbv) by day of week.
26
-------
6 CONCLUSIONS
The Louisiana data offer significant insights into the patterns of atmospheric con-
centrations of volatile organic compounds. However, our exploratory analysis leaves
important questions unanswered.
The distributions of VOCs at Baton Rouge are characterized by an impressive varia-
bility. A large proportion of the hourly concentrations are recorded as zero; many
observerations are in the range from 0.1 to 1.0 ppbv; and several observations are in
the thousands of parts per billion. In most cases this variability can reasonably be
compared with that of a lognormal distribution. This comparison can be used to give
a rough idea of the probable maximum hourly concentrations over the course of a
month, for example. However, without a better fit or a theoretical reason for the
distribution to be lognormal, there remains considerable uncertainty about the
general applicability of this technique.
Peak hourly concentrations for a day are fairly highly correlated with average con-'
centrations for the day or part of the day. This suggests that measuring, say, 24-
hour mean concentrations will give a fairly good idea of which days have high peak
concentrations. However, it would be very difficult to estimate the magnitude of
the peak concentrations from the 24-hour means.
Temporal and meteorological patterns are evident in the data. There are significant
daily and weekly cycles and wind direction effects. However, these effects account
for only a small fraction of the variability in the hourly measurements.
We have thus analyzed some of the variation in concentrations of volatile organic
compounds in ways that may be useful for various purposes. Our understanding is at
present limited, however, and we must conclude that these concentrations have a
quite large unexplained variation. The peak concentrations could be studied in
further detail. It would be useful to know whether these individual hourly peaks
coincide with identifiable combinations of day, time, season, and wind direction.
Statistical classification techniques could be appropriately applied to this problem,
rather than the analysis of variance techniques that were used to study average con-
centrations.
67 1
27
-------
References
LADEQ. 1986. "Quality Assurance Project Plan for the Monitoring of Volatile
Organic Compounds." Louisiana Department of Environmental Quality, Office
of Air Quality and Nuclear Energy.
Ott, W. R. 1988. "A Physical Explanation of the Lognormality of Pollutant Concen-
trations." Annual meeting of the Air Pollution Control Association, Dallas,
Texas.
Permutt, T. 3., S. D. Edland. 1987. "Statistical Analyses of Hourly Benzene
Readings." Systems Applications, Inc., San Rafael, California (SYSAPP-
87/157).
Permutt, T. 3., M. Moezzi, A. B. Hudischewskyj, and C. S. Burton. 1987. "Statistical
Analysis of Concentrations of Toxic Air Pollutants in California and
Louisiana. Systems Applications, Inc., San Rafael, California (SYSAPP-
87/131).
28
8715^1 2
-------
Appendix A
SUMMARY STATISTICS AND LOGNORMAL PROBABILITY PLOTS
-------
o —> a T> —3
co o c — <*•>
_- LD «r m
— C71 O CO O CM
_ CO CO CO CO CO
a z z z z z
— 5 — 3 — 5 — 5 —>
o o o o o
o o o o
CM
CM
sea" s* »« »« *«
O-. ^r> o o un ~-
CTi CT' CJ^ ^™
1^1
—• CO r^ O O O CO r
Z CM ^— CM *
< O O
ZCr Z O- Z uj —
O CTLu
>» a* »* »« w z i o
Or^ if) CO '-O CO OO
'I — O T —. OO
— u-> • — m 1-1 o O
Z A A
CO CO
o oo
r— C£ C£
O CO CM CO O <7
CJ1 i^ • T —^ CO
.-~N O • Ol
O 1/1 Ps* CM L^l
CM T —i U5 O
-------
o o uo o ^
CD CO CO CO CO
Q O I—I C£ (_> 2
— uj l-J < l-J =£
=5 CS X Q -1
Cl CTi O^ CO —
csi O CM — —
i— CX O (-1 <~1 •3-
uo • — • -sr
_j —i 03 r j co o
— cr> c^ — tVi
^u CO CO CD CO CO
^ z •z. z. ^z. •z.
— 3 3 r> Z3 :=>
-D -3 —) O -5
CO o o o
CM
zoo
»* »s >« *« a*
CT\ tn O O i-n
l— OCTi
2 Cvl
X O Z
' ZO- Z O- Z i-J —
O in o in o *z <"*"> o
O r^ m CM ce O-Z
fM tO r-» o o
o 03 o • in ^r o o
o <-> — T 01 T oo
A A
CC 23
00
cs ce
z o<*~i in m en *3~ coo —
Cv "^ in ^*f^ CM • in —• co
-------
CO CO GO CO CO
Ol-J Z C- I— Z
— >_i 3 LU ._) «
o
CT*
O>vOO
uio
CM •
ao
O
^O t—' O CM O O
O I— CM u^ ^ O O
O— m CM CO m OO
—- LT) * LT1 LO ^- .
in to co ci en
CM Ot C'g O
— i_ CQ CD
z 3: c; tx u-i CL oo
v. 33 < 3 vi i— ct a;
— o^, VI > ^ LJ V)
Z Or^
o --. en
z o -o
:> v
3 z
Z 3
<£ O i—
wj r— ^1
VI (Vi
-------
O -C ~~ O ' ^>
CO CO CO CO CO
o c£ z z >— z
— < =1 3 LJ <
X -5 "3 O T)
CO 00 CO CO
z -z. z z
—5 — 5 "5 ~5 -3
c o o o o
2
O
•-n o '—i ^i
co —i :M
zoo
Lf> O
^^ 3 Z =0
vn _i = o
uu • o O in — o s« <_) ^~
— . . ^- . . )_
I— O— . >£>— LJ Z
z .n o ir> z 3
< ^. _! — O
3 1^1 (_>
Cr - ui
x o z
L3O-1-J
** ^* >3 »3 «•? Z ' O
•O ^» CXl 1^1 CO fNJ —-• •—"
U1 • LD r*^ • rn O O
O <-n O • n T o O
O CO to m O i^. OO
o
o
: < O Z A •
— h— (3 32
: z ce cs LO o o o
13 < 3 ^) *—
u^ n c\j ^i • t^"i •—«cr
CO ^3 ^~ in ^^ r*"i Lfi co
O f^J co LO rn • • rn
^-« uD 'C' • O O CO CO
3
O u-
-------
CO CC CO CO CO
O Z Z of C£ Z
— <£. < < < <
— — O Cv
, — CO ^ ^ fi
CO — O O O
COO O
i CO O O ^* Lfl O
i— co *^" «—" O CO en
z o o
ff**s
O i^">
Oi^
C-J O ^— CSJ — —'
O • rn u~» O O O O
mo CNI co o O OO
— CO • • in CP OO
— o co o — —
in o O o
o ^" CNJ <=r o
< O Z A A
— I— CO CC
2£ C£ un O OO
o ***- ^r co T f— LOC^JCO
"^1 O O • r^*. O^i CTiOCO
— r^ • — CO O
• CD C7^ u1^ CO r
u~} c\d ^ f^ ro (,
\j~\ r^i >< ^~>
O Z < 3£ '
O w- v*i :
vi u^ o t i i— v
-------
O O O 1C O
CO CO CO CO CO
a as z z or z
Z T "3 Z -3
^r m ex, o in
O *— ex- o cx«
<— — ?X| '.n *Ti CO
wO • -CO
— r\j r-i u- r^
•j u-i ^ , o-i en
z
as
-3 -5 —5 —5 —3
O O O O O
oo o -o o o o
•c en o
ii c?> in o o
o
o
3 z ca
— j => o
< O Z
C3 Z
z 3
— O
x o z
Oin o in o <^O
o r-^ u-> cxi ce es-z
i <*n cxj in r^) i— ^^ i—i
^ • CO O in i-^ OO
jcn in n 10 o oo
co co cxi cn
o
< O Z A A
<— I— CQ CD
o: oi on o oo
^ <_) 1^1 Z-Ci-
m — O O OOOl
tn •~- •—• vo ^^ ^^ en
-------
CD CO CO CO CO
— a. o o uj c.
< z z — <
r-. (—> n vC CO
— ~^ CO — T Cvj
V- .
_^ ^^ C^ ^ '— ^"
~ -1 Jl C7i O C
CD CO CO CO CO
a z z z z z
-) -5 -3 — >
O O O O
3
O
— O — O O O
.»•"> —
UJ h- O*l
=3 Z C3
—i no
*3 »*
O O
O O O CXJOO ><_i^,
t— T ^- o z
z o o z 3
< — — — o
O" t/1
O O-uj
Z i O
O O
O O
o O
3
Z ^.
r*l CO
<^J O
t— • "V.
o<^
^- 0
ro
<
—
cc:
0
r**.
O\
m
|P*1
Og
0
H—
Gi UO
O CD
r-*
O> ^"
•^ ^3-
r^.
O O
CNj uT)
Z
2
^
r-»
cn
^>
^r
0
A A
02 02
O 0
'O CO CO
cn
-------
O r~~ LT- -^ ^-
CD CD CO CO CD
o ;> co => > =3
z _ z z u.
"1 ~- "> .-I o
— Cw 01 — O
•n o en
— CO CO CO CD CO
T)
O
— O O
VI
«« >S •» ff?
O O if) —
C7» CT* Cl —
O
=£1^1 -J 3 O
<: uj < o z
> —l Cl CO O O O CT1COO => l_l ^~
^. t— oo cnooz
3 Z O . O Z =
< t^i f-j — O
—• c\j o rv> o ^-» ^—
i • — 01 ^r i-» OO
O •=• • r-~ CD O O
— 31 T O 04 OO
-^ O — ^1 •
O O -O — O
— CSJ
ca CD
a oo
^n a-t *^-LO'a>
Oi — oj en T
— o o u-i o
^ • — O "1
— en • (M
— en o f-i
-------
CD =0 CD CO CD
O Z c_ CD LJ >
— < ^ 1U ' LU O
—5 uo u. Q Z
"O CO ^O r^~ ^^
-J 35 CTi
CD CO CO CO CO
a z z z z z
— r: = = = =
-;—;—> -3 -3
~ cn cn o co
-1 C-j CXI CM CSj
— o o ~ o o
»*>* V5 *?»*»*
£-, uD O O UD — '
^ m J3 CO
h- — O O
2T *"-• -"^
* Z ' 0
O u-. o tn o < m o
c^- O r^ C7> •^ CSi O O
— «r • •». en co o o
OO r^ . — ^r oo
•—"^a co 3 o r~- • •
J Z vn L*.
3 < O X A A
— I— 3D =0
1 '33 Si in CO ^--J O 01 LT!
j C71 rn m r-s. o ex, — -~
-— ~- co Lf. m cncoo
> — r^ m O • ~^ r- O
• • • * P") O*i * ^K"- ~—
CO "•*•. ^~ i^l L^ CO ••~*
—' T •"" >sO Csj r*i u*^
O i£ O
Z < :
< ==:•
-------
«• J~. O O -^
CO CO CO CO CO
.—WJ O uj < <
•*•* "•"! CO C"i '"'"*
z
H-
^J CO CO CO CO CO
—5—5—5—5—5
CO ") ~- f- <^-
CM — O O O
- o o o o o
*^T CO CTi 1^^ O c*5
CO 'jl
O • — CO C^
co <=•
— Cj
*** ir? 4*
o O un
< O uj i— ^l
— -^ = Z =0
0£ 1/1 _ 3O
^^ *^i O f^l f^ O Z
Z !•» c^ OO
—i -y\ C5 ul CO cn
-^
O O _• CO -^ • CO O O
co Cj co un o co ^r«
•^ ~— ^— O^ CM ^3" J">
CM CM
-------
CD CD CO CO 03
O Z CO Ci Ci 5-
— < U-J < 0. <
-5 u_ Z < S
S- m CD ^O —
»— C^ CSJ CD f^~ r>i
— -O Oi
O
-j CO CO CO
— 3 3 =3 3 3
•^ -3 -3 -3 -5
i— O O O O O
a« »s
o o
CTl —
u CTUJ
2 i Q
< '"I O
QiCTZ
^ co m ^0 t^ co ^-1—
CNi • CO O • P-» O O
^•LO CTl O CO ^D OO
Cfti-f"i "^T • ^v ro OO
^ LJ on c_ O-
2: 001 — r^ co T
o ojr~. ^- o cn rn — 'j-i
3: *ro O ^r ^n c^ unr^
o *r ^r ^* m . • LD r
CO tNl O r*1 O CO
O c^i ^^ r^ C^i CO
0^:0
I1 Z
ca L_ ^ 2: < ,,
-------
vo o o o o
CO CO CO CO CO
££ — J cr: z 2
<=<==
Z -3 Z —> ' —}
_n ^n r^ GO co
— CM O O —
CM
CM
*— CO CO CC CO CO
O — — _( —j _J
— 3 3 :Z3 ID 3
—1 ~} ""3 ~5 —5
O- »*»* V! **
u o tn o O
u. CT* O"i O^ ^
mo O O O <-!OO
CO CD
Z
OO-uj
>»»»»« Z I O
C-ri O uo
O ^- tri C\j
u~i co un •—i •— *—•
rn in csj O O
CXj • 1^1 i^ C< ^)
^O 'sO ""O O^ <^*j i^l
T r^. O 03 • •
r-^. — r-^ CO
—, O
O O
CD CO
O OO
"Z C^^T C7"i <"n C?i O O^T1-^
O c^j '"") *^r O O r*^. CX f—• ^
Z ^~ c*j co co • • o en co
O CO r*i CO csj CM 'O rn —-•
q» o • ^" CO * J^
^~• 0? '-O Csj i^\ '%O CO
i— — z <
O Z < 3£ .
Z 3 '-J
< Q —J wO
-------
CO CD CD CD CO
S —i cr: —i —i cr:
— 3 —i O —« > •
o ~- ^- o
Ci O O
—I O
O Z A A
i— 12=0
ce vi a c: O
^ vi i— a; at
i^ u vi a. a.
cn ^o CM
CM J"> U^
TCM <"~]
cn CM cn
-^ cn
o
o
o
cr:
<
-------
CO CO CO CO CO
S CO CO CO s- Q£
CO CM f!
rr _-> o
CO CD CO CD CO
O _J _ —J —; —
— = = =J =J =)
-5-5-3-3-3
O"t CTl CO CO CO
M <^ rj CVj CNj
O O
•
«i~>
m
3"!
«•
O
—
—
o
UT!
Cj
C>J
O^
u-i
n
U1
^
r-^ — t
^_
O CO
^ ^r
^- o
•ZT —
(Nj ^i
O
<— t 1—^
oo
o o
oo
.
LD z un u
3 < O Z A *
— i— CO CO
SZ a: oc vn o OO
— '^-ivn > ^ <—) '^} Q.C-
O U^ CTl Lfl r^* CO ""^
^r —"^ cs CO ro p««. tn >—' CM
Cio o — «r • T T—
CM ^3 • in ^i > co
• • CM *3" r-^ CX) ^
O ~- CM CM r~, —
-------
03 CO CO CO 03
— = < O O l_>
—) 2 Z Z O
— o — — :*
i— TT CO T -O T-
i_i s T co — ^ i-n un
• o o o o
< Q
ce <-n
> JTCMOOO ^-OJC
Z I— T O T O
co ,-. (si o o
Ol Or-. O O
O°* CNJ 'O ^1 C^
o co c^ — tr
— — r- o
3 < O Z A f,
— ,— C3CO
zs ae ct oo a oo
i— 1^1 vn > ±4. '_) on o_c»
^ c^ ^^ ^*- f^^ -^ co ^ ij^"
O ojr-j un Ln CTI cri ou">c
O CM o ao en • ^-
-------
*a u") O o o
CO CD CO CO CO
O =_ •_> > Z >
— —j uo O O O
l/l C Z ~5 Z
CM — ~^ o ~-
I - 33 t*l CM —
^1 . —.
'— -O O «r
~ — CM
o
u-i O3 SO CO
~5 "1 —5 -0 -5
CO CO CO CO CO
T »S 4-5 »* »« »*
'i o tn o o o^
CTi ^
« o
O£ 1/1
< LLJ
mo o O O moo
X O
i-n -•>
Z T ^w CM •—
O1 CO sC CO CTl O
01 p*: m CM
»— • CM Oj CO
o o <=• — —
-------
r~~ O ^O
CO CD CO
Z Si Ci
U_ U- "~3 Z
J1 O CO 'O
o o o o
i— o, CM ^ m
VI •
CO CO CO CO CO
i _i — —I — _!
•3 = = = =3
—> —1 -> -> —>
CJ"i Cn CO CO CO
CM CM CM CM CX
•S.
>
»<***«
O LO o tn o
O'— u~> <^
O CO CO CM SO
'"*") '-O CD CT^ Cj CO
'"I • ^—
ro CM
OCO
cn —
. i — .
=; ot
3: z :
-------
CO CO CO CO CO
• O ' ^ t^ <_j
< o < z o
- *r> rn i— o O
T . . . —
J O CO Of "^
i_ CO CO CO CO CO
-3-3-5-5-3
•Tl Cl CO CO CO
— O O O O O
— -o ,^j O O O
o o
*r
ii OA -n o
L^ CT) C7^ CT^
O O
x o z
<£ —1 UJ — —
zo- z o- z
^ CSi — — •
<-1 O OO
o o oo
«r o o
o^ o co ^
o ~ co o
o
V5 LiJ
O Z A A
i— coca
e£ on a 30
=> o-, — ce=£
^ •—, -J*. Q-Q.
f***i fSj ^« iO '""
z •=• ^ oo co
—I O - — OM -O
o rn — en co o I--
O • CSi --L3 n
VO 0-. C3 _i — UO Z
-------
O O 1C iS O
ca co co cc co
a >• z z z >•
— < 3 3 =1 <:
2: — ) —. i -3 X
o -- o ^ —
"1 ?,, CX. O ~
u-i co ev.
CO CO CO CO CO
_J _ _J _ —1
=1 = = = 3
-3-3-3-3-5
„-) J^ in — •—
^, Cj C^ C^ ^
O O O O O
3
O
~- -3- LT, O O O
^r
M O 01 O O
O
U-l
U.J
—1 010 O O O LOOO
3
o-
V! 4?
o ui
o i^-
en— en oo co o —• —•
— < i— t^-t
O z V-: utj
3 < C Z A A
— f— =Q CD
ZZ et: cc iyi O oo
O t\j— o O • — cou-icr.
co —• '^ — • o
• • O 3
— !.-l Z
-------
o o Ln o o
CD CO 03 =3 CO
C£ 2- i— >- cr:
c. C-, '^ CO ^ O O O
Z A A
co a
vn a OO
V) '— C£CC
^j
O -i m ^T <3- "^ CTI O O -"--I
<
— z
< i—
:> z z
*^ CT^ -^ • ^ O ^
CO -TO •*--.
o o co m o
o ^'.
'i Z
z <
-------
Q.
o
o
o
ca
o
O
CM
O
o
-------
O
C^
O
O
O
;/•>
O
O
O
-------
Q
O CO
< l£
T: =1
uj O
3
cn
O
O — E T:—
-------
O rsj
O, C-
un oj
a
o
O
CD
o
o
O '_ E "3 — <^ u
-------
o
o z
o
o
Csl
O
CO
o
-------
< a
o
co —
—3
o
o
O '_ = T3 —
-------
<
<
<
=2 <
0
O
o-
o
•^-
o
o
o
O i. £ -3 —
-------
CO
o
a
a.
o-
o
o
=3
O
O
o
o
CO
-------
ivj C£
"••sj
^*i ~
•O
O X
o
o
. ^
o o
o-
o-
z ca
O
o
CD
O
o
o
-------
en
< 25
I U~)
-f-
t O
O
o
O
CO
o
CXI
O — = T3 •—
-------
<
<
<
u
< :
<£
O
J O
z
O '— S "3 —
-------
CO
cc cs
a:
S3
O
o
en
3
-------
< <
<
CD
CO
CO
ca
o
o
o
o o
CT
o
o •_ E ^ '— vi '.j o - CJ
-------
ca
LU
CO O
• CO
L3
O
O
O '— = " —
-------
o-
u-i Q_
O
O
0 '- E •= —
-------
•a
CD
•a:
O
o.
-------
o
o
-------
et
CQ
CO
-------
< <
co <
<_> <
O
ca
ca
-3
j a
a
.
Q_ i tn o
0.0. ' O ^
LO
O
(/I
O
O
O
O '— — "3 — vi '_< O '—
-------
•J
z o
3.
X >_>
CO
O
o
o
-------
Appendix B
SCATTERPLOTS OF DAILY PEAK 1-HOUR, 3-HOUR, AND
8-HOUR AVERAGE VERSUS DAILY MEAN CONCENTRATIONS
87 1 Si+r 1 1
-------
SO
O
VI
o
••3
CB
O
ce
0.
-s
—
o
-•
o
c_
o
LTl O
a.
H- Ol —
i n —
i -a
-i- 10
ca ca •*• r-.
: < < i c\j
< LJ < i
< ca
—i ca ' oj
ca
-------
ca •_> =3
ca ^ .
«t
-------
v-l
CO
O
— O
•S 01 -
•3 ui i =
CO I fs
— O i _
l/> I 3
•C II * O =
Ol i CO
•= <: i a)
**•* i CT*
O Z O i -I
- — ^. I
•^^ h- uj i
<3 O O +
•o
o
z
l«i
5
=3
O
o
>—
O
<
<
< < O =>
< CO -
< CS :
: -5'
aj •_ f^ 3-, aj c: i^n-*-j-3 —
-------
CO
<£.
1/1
22
C
C^ CJ — i^
-------
<
0
G
—I
a.
0
o
0
o
CM 0.
CM
o ^
CM •_
01
>
co >,
C2
O
«* « <
- ca
« i
< < ceo:
< < <
_j ca
03 + kO
O UJ
CO O i
en o
« u '.j -r ^r
<£ _l Q
(_l ~4 * CM
r 1 rx,
CD f^vj t
0
o
-------
o
> O t^ —
i O ID
+0
-I- O
i CD
« <
-------
•j
— == «t
— -u
r: ^l «t
•a z
—i
• -•>
CO < i
< en i
< <:: aa—j - O
< SO uj
< CO _J
.o o o o
O O O CD
u-> *r rn cj
S^^ <>o z ^rc^-_ T;>
-------
03
O
ca
o
< :x
-f- LO ' —
i a
i -O
*T*
U- J—
Q i • '
-*~> U_
c o
~ o
CQ < < <
CO
-------
O
.3
-------
l/l
33
3
<
ss
.0
cc
O
O
tfl
O
o
O
o
O
o
O
o
O
o
O
o
O
o
O
o
-------
O
Q
o
CO
o
o
o
o
CO
o
o
o
o
r3 > OJ — (Z ^">
^ -^ — O 5 C ^.
-------
CO
o
CO
o
O
Z
IS
•o
<
o
—
a.
a.
u_
o
C22 03
ec
CO CO <£
CQ ^
<£ 3D < <
cc s u
L^J
<: a —
C2 O =Q
<
-------
> LU
<. —i
o
o
CC
U-
O
i _ -: 01 o
o
CSJ
C ' .S 3 -
-------
CD
O
r= O LU
Q-
O
O -
CNJ '«
CD a
cc 02 ca
ca <
-------
CO
O
O
CTi
O
CO
o
—i
c.
co OD a:
CQ <
< CO
<
-------
<""•>
O T Ci
— — a=:
4-j h— uj
f-3 C3 O
*rf
-------
-3
O
O
O
o
CO
* o
i O
< <:
«Z
<. ^ ^ "~ ^ f' *~ "_'
-------
•J-t
o
CXI
o
z
o
-------
O
>
<
O -=1
O
O
< <
«
< ca
<; co
-------
v/1
C2
o
-------
O
en
ae
CL.
•3
i—
O
—
o
-------
o
C-.
ca
o
O
O
o
c*^
O
o o o ^ rz
- = CD O O
co o •=• rj o
-------
O
o
O
o
a:
CO
c%.
— o
^ > a- — ^: c*.
vO
= O)
-------
OD
ii O
z -z.
— L^
t— '-3
> _
<
•». oo >,
z
cC
z
a.
O
O1
O
OD
O
O
O
un
CL O — — ^ C CJ
-------
OJ
a.
32
O
O CJ
-t- O
i m
CO
<
< < <
« ea
•S
~"
ca cm
<_> w>
<: ^
o
CD
> o '— 'C
-------
<
CO
> 1-1
< —
<
co
i_) O UJ :_!
<: LJ o —
< co •-: <£
o ^: i_
< ^J Z uj
-------
4)
O
CO
O
0* <
C
CO
- M =>
C X Z
— — -J
_ ,— U
_i
— «
=
OJ
U
= -x.
e _i
r= =1
•c — i
O
>-4- «^
O
CO CO
<£ ca
<£ -a: u
<
o o o -
CO u^ CSj
<; > ^s w_ ^ z ' — o z: — <^ >
-------
-II CO =~
TI < i —•
cc
D Z Z < 3^
C -J — ID
3> _J I >
- «C rs
U i >,
= X i -
«£
<
32
<£<
< C2 <
< J-
O
o
-------
o
c
50 <
< 23
< CO <
<: Q -o — z
O
O
i X 5- _| _
-------
<
•s
'•j O
< O =-.
» o ^
i O
-t- C3
< < <
< e£
«c -a:
=r i 22
i o c
CD <£ < * CM
i •_ -s o-. i — o — t: -— ~.
-------
3 Ln
O S3
— O
- '— j
o _i
o =
< LJ
3 > <
= 0 <; so <
) CD •-_( Q < i —
: cc u_ <: z
co o ee ' n
< Lu !_l I O O
: <: u~ • —
« W.SO i — =
< < o -j i on
: L3 — i -n o
co — u. CL -
cc — ^ o o
-------
rs oo
o cc
— o
cu z
Q. ' - J
(_3
'_ _J
O —I
CU _l
> l_l
o
o
O JT
M O
< <
-------
=0
•=>
ul
_i£
ra
<2J
en —
-------
.=: o
G
<
-------
O Oj Z
— ~ O
c/ en ce
c. CTl -t-J — — ^ J^ — O — O1J — J^^— 1) — O>
-------
= cs
o
=3
O Cj
O CJ
— Q.
O
O u-i
O -i-
CJ\ o
fa c_j
CO
•
O
-------
=-, -— ca
~ W~;
O S
.= Cj
c
O
•o
I—
o
-^
o
CO <
CD O - —
CC « =C
-------
en
c
0.
o
o
-------
CO
o
3
O
** I— C3
IB O uj
— > _l
,3-
o
O
O
-3
CD
< < a t_p
ca <
co «£ < <
CO O .22
co
-------
O
<
< o 10
CC CQUJLJ (_l
ca •_) LJ o
< =SUJ X
coc; u_ z
O
O
CSj
-------
3 VO
O =2
^r o
1/1
-*i
15 o
oj z
d, -J
O
— uj
O —i
OJ
tx.
en o
o> ai
> O
o
O
=3 <
^J
— 5 X C
'_- ^: — O - G —
cs.
o •- =
-------
n; u"i
— O
o
c
o -— u.
LJ QC
01 O
> O
rs u_
C£
0003
in ^- n ^4
O 3 •_ -:>cn 'j ^ — O '_ 3 — O - =
-------
<•=
01
O h~
w O
CO
O
VI
O
'_ ^ .— C— '""O-
-------
CC C£ — CO
c3 _ i o =:
-------
<
<
CO
•X
<
CO <
=£
< «
< «
«I
-------
O =2
.= C3
C
1)
<
<
en —
* . c O
«Z
<.
*t
< <
O1 U-taj^I
-------
13 uo
O C2
a O
O
=
0)
o.
O
u_
',—
V3 L—J
O
O
p
a
i —
LT> .r:
•_,
O —
•X.
<
3D <
« «
. SZ <.
-------
cc
o
O
W-
0)
— LJ
en a-
ra c.
*_ -it
0) —
> I—
C.
O
O ~
r-i -a
o
o
-------
CO
o
o
e
Oi
£
— X
O
O
<
'<;
-------
C CC
— o
en o
10 —
O
o
— ^r _j
c-j 01
—1 >
-------
<
<
O 1) Z
LT.
•>,
O
O
-------
O "~
^J i
Oi
co >
•o
CQ O
<-J O
CQ a u_
CO <-J (_)
CC U_
— o — —-
o
U-
4)
W
u
Hi
-------
•3
O)
O
O
cc «: <=c
32=3
<; CC OL3 !_1 CO
O
O
-------
<<
,— OJ =
•o — ^ — — o u — -a i/
-------
•s <
Q. 13 •_)
CO
o
03 <
-------
•J
u -u
o —
: C"> -x.
i. f3 h—
"i £ z:
r r
j
i
<
< < =0
< <
1
< _
o o o o o
' — O - — a>CH —' — •- w « — o —
-------
< <£ '
< ca
•s
O
cs.
CD =1
« c:
=a •=;
<. <.
: < •
<
-------
— VI
O CC
— O
a.
o
<
-------
o
:M
CO n
~- ca
1 Q
u z
Q. UJ
O "_j
> o
« «t
.— LJ
< LJ —i i
Q u L_ •>• -n
<; oa -j ca i
Oi_ i-j i
CJ IE 23 I
< <_> IT ca i
< o o u. * c^j
ivj - O
o
o
-------
. r-* r**. LT> LO u~t
CO i"*- O O f^»
» *^1 CT^ fM r*^ O — J i-H CT" C\j Og u^ O^ O^ O^ ''O CO fSj CO
a u_j mrofoncNjmn O |-O co co vo r*^ o O^ CO co o^ ro
C Ct ............
-------
_j ^r
?: an
iyn o
O
uu
UJ
O
O u-i
O CZ
CC CO-
utj ^r z
z i— —i <
—; < Z
uj i/n
—i «t
i^j
z
00
co
co
o
an
uo
O
cn
cn
O Cn *T f-^ CM
an co *^r *T CO
f^ ro o an in
O an o an 10
r-~ an •%. ^r —
e-^ CM "O CM CM
iO cn CO *—* an
O an CO O O
O r^ ex ro CO
00 — '0 — —
O
CM
^~
O
o
^__
cn
r^
r —
O
en
cn
an
0
~i
>^p
*T
<^-
r-^
CM
an
CM
o
o
an
O
CM
an
an
O
r-^
rn
10
CM
o
~
o
00
e;
o
~-«
CO
— .
O
0
CO
ro
0
CM
'-•
0
o
o
f-^
CO
o
=5
CO
Cj
o
CM
ro
CO
0
an
f^.
cn
—
O
CO
•an
CM
OO
«^-
O
O
o
o
^
ro
CO
cn
CO
o
an
—
^
^
~-
u"J
~~l
CO
CO
^~
r^.
O
^
CO
r^
en
CO
ri
cn
'*"
o
—
CO
ro
'i?
o
an
CM
CO
r^»
O
o
o
"1
cn
ro
O
O
an
ro
-
CO
o
=
o
o
cn
an
— •
an
o
j
CO
o
5
~"
o
o*.
C1^
o
0
^.
'::'
Csi
vD
an
r-.
cn
en
r-»
~-
"
O
an
cn
O
1 — .
an
an
^-*
O
O
en
o
cn
ro
•3-
ro
cn
CO
CT^
^
cn
un
ro
un
e-^,
r~^
«•
0
r*x
CO
rr
CM
r^.
ro
^r
O
un
<^
O
*^-
C"
0
en
—
^«
0
0
—
o
o
^,
o
CO
cn
' — '
O
an
r^
'fc»-
O
en
i^
un
C2
CO
ro
CM
r*.
O
O
r-.
—
O
wO
r-^
^*
r^
r^.
CO
^~
O
o
o
r^
CM
an
exi
an
ro
—
O
O
Ov
0
an
CO
ro
cn
CM
—
cn
an
ro
O
CM
—
O
•~^
CM
ro
exj
CO
~
o
^
e-^
0
.--^
ro
O
O
o
-_•
^o
ro
-
an
CM
—
O
CO
—
=
^
o
r-*
CO
r-*
O
O
—
0
un
CNj
C\J
LH
CM
C^
i-^
O
0
cn
cn
^T
C*-J
cn
Ul
o
— '
—
Cx,
^
^
"-v.
.—
^*
^r
CO
o
-—
o
^~
—
^*
o
•^r
O
CO
-^
<>J
r—
CO
0
-w^
r „
O
u^
O
o
C3
O
^-,
CO
rr
—
«^-
C J
OxJ
^
CO
r"
O
^
O
«^-
a-:
CM
1*^
,_
—
o
CM
CM
f^
ro
cn
^^
O
o
o
1
^
an
0
O
O
CO
o
—
o
ex
0
—•
C2
rr.
^
.— >
an
O
CO
an
an
O
ro
en
cn
— -
^
•^
r*~
cn
—
-
r— 1
--.
^
r.
CO
TT
o
CO
cc
„-
—
—
— ,
-I
^,
cn
^
«r
c^.
r^
cn
_n
LTi
0
n
—
-^
o
ro
^~
rv.
CO
O
cn
o
0
o
0
1^-
CSJ
O
C\J
^~
0
C^g
O
^
CO
^
^T
cn
cn
o
cn
^
r*».
•-r.
cn.
o
l*v.
r"
•^
O
Oj
O
u*)
-C
0
^
CC
—
"^~.
_r
^,
•^
—
—
T_
^
^.
cn
r »
c ^
r-^s
" _
^
-0
°
^^
Cn
e^
^o
—
O
3-.
—
0
ro
U3
CO
r-*
an
ro
0
O
CO
—
•an
an
CM
O
CM
—
-
^
O
•tr
<^-
cn
cn
cn
<=•
0
o
—•
^r
s_T;
^
cn
cc
_*"
r_.
LD
f—
/•*•}
^
3
^
*
c^
•**
~
^j
O
o
—
-V,
""
-
~
CM
—
"^
^
—
=
'"'^
cn
~**
<^-
i™*i
u")
0
o
.0
o
—
LO
OsJ
Ul
o^l
O
O
cn
• —
^4
O
cn
•~^.
'-»s
—
0
^__
cc
CO
"-^
«T
_i.~
2O
Ox,
c^
^
cn
ex,
0
ex
r"
O
--.
rf~
O
CZ-
^
~"
~
^
r_
^
cz.
-n
_~,
o
cz
cc
^T
~
-
CO
r*-*
~*1
"*
^
^
—
^
~
^,
O
r^-
—
r^;
—
0
O
^
O
^
r^
«r.
C-^i
O
0
^
«•*,
•^
'vj
f^.
o
o
—
-
_-)
'-"1
-^,
_*
_-;
-^,
~*
CD
f^-
o
^
•—
„•"
_-
o o o :r
-------
CO
o
o
o
o
01
CO
5-
CT1
t^
Ol
3
•xi
3
-------
. Z U"} UO U~l O^ CO <—• i-H
J < *r CNJ f— ro rr "-«. CO
UJ CSJ CO <—' O O •""•• UO
3: UO —« » ^ "*-. r-*
'""•"• CTi
O"* O c\j ^J o <
ao r^. co rv. co co en
C£
O
O 00
o- <
UJ
oo X
I
UJ U"l
O Q£
Z <
O-
-Z O CNj O — f*^ O O
i r-^
UJ O O *T LTl uTj C^ CO
3E — « C\j r j O CO — CTi
GO ^r co — c^ <=r <-*
CO O*> CO O^ O Q"i CTi
^O O C\j *-•
— • o c\j c\j un un
» cn o co T 1— cn
<
LU
•Z
tjO
rv O f*^. — m <3" r^
an o co ^-. un cr^ •— *
ro ^O O «r CO wv r
csj •— ' o C^ r*i f-*.
rv, r*x GT\ 'Ch CO *sO f*
<; r-s. csj o m o r*^ c\j
u-i CO f^ CO *—• O O CO
x t— en <-"> r^ cr» o co
(/i co •—* 1^1 <^ CNJ vn cr»
—J U"! C-J !^* CT^ "^
m ro r*x C71 P** O O>
CO CP ^ O U^ C\J r^
Of— r
— O r-1-- *T C\t CNJ r
O CO i — r-x r*^. p*».
N O f*^- CTi CT*>
co —• (--. — c\j cn o
r*v ^— CO CO ^O CTi -=r
co ^r — • u-i ^n m co
<-> o «T co ui o en
CO -— CO CO
T tr un un
ooooooo
IT) ^- CO <
«^ cr> co rn m
en *— m o o co oo
CO O CNJ r-v r^ «T CO
^ C\j CTt — CM f*O T
C\J CNJ *-* C\J C\J CNj CNj
O Z CO CNJ Cft <-^ m ui Csj
i — i < LO vO •— • r*^ ^" CT> T— •
_j uj r*K ^ LO — P^.
U1 CO ^- *O CSJ CO <
uj CO CNj LiO CD *""••• O^ O^
Z CO O r*^. c\j — *c- LD
uj CO U"> "^0 '*^ ^-- CO —
z cn co (*•» o o ^- cri
f— ' r^. CTi ^ CO CSj O
ocnocnoo o
j CO CO i— • CTi ^n CO
O< — —• -n
> uj U~l C\j O
LZ Cn O O
ii on 'sOco o-i
z _: o^ocr^
^ r") LT> "-)
o sr -n
OOOOOOO
— -— Cxj PO <
. !
o
-------
o LD CD fx. —• uo CM — -
'O CM — co — CD -=r co Oi O
5 — —O O O
1OOO
D Z O r^- O '"I '"-*'—' CT> <3- ^ *T CO i-<">
j< CM — o co *— '~r> CM —
^..i ro "^ CO ^* U"> '"O ^NJ r""-. ^i •—• CM *^T
X -srCMCMCO — ^^"COCMrv.ulcO
oO CT> CO ~~ <«O CT1 *C7^ 'J""* CNJ CO CT^ *~O r^--
'CTiCO—-T—-CM
CM O O — CD «T u"> CT»
^ f^J *~" ^ C7* >-^ '^i CO CNj CSj C\j
— t — i o r^ uD CTi O"* CD CTi CO CT* O">
— • — • CD ^O U^ *5T CO «— ' CSl O*i ^T *^O
f^OClCD-— •rocfi^CO'— 'OCO
CO <""> '-D ^~ LH uo CNJ ro r»» O ^o c\j
— ro CO •— '
— O
— J O r^ O O^ CT
.— r*. c\j CO %O O O
^r o en r^ o co
f^ CD I«O CT* '"^ ^^ CT^
*— — r^ O CO O rn
^TCNjCsjcoo
^ CSj O"i UO CD CT^
r-v.cNjU'icsjrorn
J Z PO ^— «
. O — U-> C\J O CO CO
2E uo i— • r-. CO —* —
r**. O ^"^ r**, \O *^ O
»— f— — O O CNJ CM CNJ r— »-• cvj CM
o cr> ^ — • — tn co CD — o co — •
^ro — o — TCOro — (-03^ —
3'*U~l CM i—«
'-oo — CM-CTO
^-rsjroi—«OO
o CT\ '
O CO CTl O ^P CM r^ ,— CM CTi CM O
OOOOOOOOOO— "—
OZ O i-^ ^" rv. u-
CE
' CO i— • CM O O uO CO ^ CT> J^ rx.
— CO-OO
^- — — o~ — o o o
OOOOOOOOOOOO
— — O C O 3 O
-------
< CO
uj GO
X 01
o o o
O O T
00 —
at
a_
o
o
o
o
*r rn ^ CM
Oi O T —
I-** fl CO O
fM UD — CO
O O CM O
O CM — T
f"> C\j CT1 CM
o
o
O
C£
o.
U-!
UJ CO
o; o
-------
c
UJ
LJ
O ^"> LJ Z
c_ < > k— mr^ooooornooooi-n'~(-^'^-'^"^JO^OOCOLn OO '*'*. *••* ""^ *vT '"Zv CO f*^ *O ro CNj •*•«, CO CD "* "~j i/*> •"• r*».
^ ^" O '^ O O ^ ^"> O O ("^ ^J CO (^^ CO
j CO ^* I"?*! 7SJ VO f^J ^T CO ^-O ^ *^ r^ Ol
oo; ........................
S <. o r- 1 n con m n m ro «r ^x oj csi O T
o
5»
I
^ O — . e^ n «r un o i — ^000^*— — -^-- — •• — •— .^-^-r— — .CXJCNJCVJCNJ O
e^iO^— OOCOO' — r-[ ^ — w-^~
u*> .^3 CD r->
' — > n o t~n en ^i m — co
CD •"*".
-------
Appendix C
ANALYSIS OF VARIANCE TABLES AND LEAST SQUARES MEANS
371S^f1 1
-------
O-
O
en
a.
VI
a z
o —
o
CP
•— UJ X
*—• vi _J O L*J
z co _j 3;
o o <
i— ce —i z
01 < < <
> -> T i—
co ce —i z
vi
m
o
o
cc
uj
CO
z fi a.
o
z
S3 UJ
O — uj
o o — —
CQ
O
C^ Li~J O^ ^J
f*} O C\j —
—. o ^- o
O — csj m
cc
O
— O C < C
uJ — 3 a z
o
Oi
o
-------
o
CD
o o
o o
CM CO CM
CM — C?i
o-
C£
— — O
CD
O
•sr o o
CD — —
o
o
CM CD
— 0
O «M
CO
0
o
o
O
o
o
O
O
O
o
^_/
o
o
01
o
CM
cn
O tn
— LO
o
— u.
Q. O
CM
CTl
CM
CM
O
o
CM
O
O
o
CM
UO
r*.
CO
co m en
CM CM p^-
T •— CO
«T O
O-i O
in
o
o
o
>- 3 Z
O =
= 3
-------
o
CO
cc o —
LH co co
< CO
= O
o- o
O r^
o o
•c- o
~- CO
iO CT>
C~. Oj
cn o
O
o
o
o
Q£
CM
O
O
O
I—I ,—
co
-------
— e:
r--. —
-3 CO
— CO
cs. -3^
\ft 31
^*l CD
CO —
r-! CO
~- CO
O
O
O
— 01
"1 O
O "^s"
C£ CO
O
O
O O O
O O O
O O O O
O O O O
O T r^ •ST
ro CO CO ^1
O
Oi
O
O
CO
O
31
Ol
O- —
O
O
(NJ
CM
CTi
O
-------
— <;
co _
o z:
C£
Q_
Ci -1
CO (-» O
u-i —
O so o
— CO vT)
— cn
o o
o •=•
O — 1 T —
GO
o
o
o
o
o
o
o
o
o
2:
S£
z 01
<
uj O
CO Lfl
— n
^j CTi
CO
o
<^-
— .
l-s.
CM
un
•^*
^j
GO
^r
C\J
r^.
U-i
CO
C^j
en
o
rr
LTl
u- *
CL.
>-
i~~
i_n
«T
*^
0
—
CTi
O
•cr
CM
LO r*s.
CO un
«• o
T ^^
r^ «3-
-------
OJ
•s-
o
o o o o
0000
'-O •—
, — u_i CC
CO r*s. O"* ^^
O CTi CO C*i
— —. CVg —
— —'
o
o
'-n G^ -f
ro o «T
CD
o
O
cc:
O
O
o
O
o
o
o
o
o
o
o
o
<
=
O-
CO
O
CO
C">
o
i . i O CO
< C^J
=> r-.
GJ O* O
D fsj
•vj t__ .
= 0 O
O f~-
co •^-
^— n
co co
^ r*",
CO J^
o
C7>
en
o
CXJ
en
O
CM
rn
Oi
O
CSl
en
co
-------
Ol •— O
co z 01
O
O
st
a.
CVi CO rr
o .~- o
01 co in
O O Ol
LT.
cn
co
co
o
UJ
UJ
o
CD
cn
(51
CSj
OS
Q.
O
O
O
O O
O O
O O
-------
:>
LJ
CO
> l_
^ O
o
co
CO CM
CM en
CO
CM
co
o
CD
en
en
o
CO
1^-
C-J
-------
— CO
o o o o
o o o o
— «T
o
o
uj CD
O
O
u~i
Oi
^T
O
0000
0000
o o o o
CO
LT>
= o-
OJ o*)
>t u-
X O
tn u~»
T O
O O
rj ^3 ^o c^
O rn O T
CO
O J1 T
-------
33
CO
<
CD
o-
V! O
— co en
— — co
co o
ci co
o 1-1
o '-*">
co u"i
O
o
cc
o
o
o
o
o
o
o o
o o
o o
a
o
3:
O
CNJ
u->
o
O CTi
— o
"• O
— o
< =
Ci O
O u
o
= o-
3 ^
O
o
co
CM
O
csi
-n
CO
CO
01
co
01
en
O —
o -;
o en
cn
co
o
CNJ
<
•f
-L. C3 •—
LJ =-3
Ci • C£ ~
O C <
~ 3 Q
-------
—' •— — o
=> o o o
o o o o
3 -n
CO CM
CO CO
o en
— CM
-o —
cn co
co —
m — .
O m
O —
OS . CO
o
*—I
CSj
<£
L^
z
o
CO
o
T
en
vO
o
o
o
o
o
o
o
o
co
CO
o
o
o
o
un
o
o
o
<
C£ I/I
O l_>
'— CC
•a «:
^ u_
— O
o
o
co
o
-o
01
O
O
O
_-!
O
O
O —
i~» —
co co
r- ^ Ol —
O ^- ^^ m
en co CM o
'1 rv
CM —
C_ =
i_ O
-------
30
cc
s d o
— -n
— co
o —
CD
r~^
O
O
c-. CM —
r— O
CO
cc
C71 CM
CM
CO CO
o —
en
<
3
cr
o
o
in CM
—' CM
n 01
CD O <—
O O O T
O O CM f^-
O <—> O O
O
CO
CNj CN.
— LO
CO CM r—
,-) CO —
c^j en o
CO — r—1
o
3:
-------
CO
CO
-~s
o
—• CO
oo O
01
r-1
CD
CO
en
CO
CM
O
O>
CM
CM
en
o
Oi
CO
01
rn
U3
r^
O
<^-
m
01
m
Q.
o-l
c£ Ct
O
o
o
O
o
o
a. o
o
o
o
o
CM
co
Ol
CO
— O
oe o
< —
3 O
C^ CO
oo r-i
CO
Oi
CO
f>
CO
O
O
o
— o —
O CO —• vO
•=T O CO —
O O O O
u~) Ol O O
r^
-------
-C O"i o co — -— ro o O
— CNJ u-i — • CM LTS c co •=••=• -- "O cr> -- cc — o co
CD 2: co— '-ncv-
— w~ co """i r-v o T CD -i
o o o c^, Csj cc -— co
CC ^ ^- "^ CO ~- 0-- -^T
— — . -^ r^, r^, o O U~, _~> CO O —
CO ^ CT" ^j ("^ "~^ CD
•—• *^ O r"^ CD Csj O
— en co o as
^. en c- r>. — era-, — oc: — o — c
•^ "**. *^r co co co in r^ cr ^w ro c^ ''^
-noc. — ococn
^mrrcoc\j'^cricr>cri
cOuO^.Ou~ir-) Ln — o -" ^-^ — X ~
O(^O"^.-^OOOu"lO*TG*'"^CC-"'''T'^C*-S
•O'—— -OO^-^J 3<^—'-SOCDCC-TC*. tT-"i—
S O O O O O O <
o ^ ••"•; c* o CM ui co — •
- o ^ u c-, o -^ ^n o c^j — - fsj •
--^ j~- u^ o -~ o sS u~ " _
— r-^ O — C1-^
OOCOOul
— or, — O-O — -*. c^ o ^
-------
O — ~— —i
r-.. r^ ~_t CM
T '~3 CO CM
ro
•o
o
Cj
— o e;
rr CM en en o-i en
,-;—•—• — o-> o
-si cn en T eo co
— — eo d -i
en e~ en en -o
CM co «r — -I
.—i co r^, in —
eo
co
r-i
LO
CO
O
o
co en — --
m O en —
en — ^ o
CM "- co r.
o o eo r;
co —
eo m
co m T C r^ CM _
co — co --i eo — -=r
co <=• en ~- ~->
— — en en -"
o en o-i ^r en
en co r-i o en
*~^ c^j r-*. T en
CO -O
co en
o —
CO C-*
co >n
T* -^- rn £y^ - _ r*i"i r*-j 20 ^T **T *^~ -"•* ^
— O-^r^O — •vT en — eo CM ^r
CO —> —- CO O CB CM u-> r^ C3 "~ CM -^ —
^ CO n —
cc o en ^*
O m -r- in
O O O
! CM
0
m
<— 1
) en
i ^
r^
• ezi
> O
0
,3
U~J
CO
'"H
r**.
^_
O
O
r\j
^r
r-.
er
rn
en
0*1
r*«,
— .
un
•^n
cs,
O
— •
en
r*^
o
CO
CO
P-.
r^.
—
O
O
_
1^.
o
__
CO
o
T
O
C^j
en
o
o
en r^-
en —
en . O
i—> CM Cn r-x
r^i in *t~> in
— m cn
cn — —
co CM in
n cn CM
— O m
o co en
en ^^ in
o en
co CM
CM -^
in :M
m co
cn n
o •«.
-o
o
en
o o
z <; •a- cn i
i_ u. CO T i
en "i
Oj
CM
O
<-")
CO
«T
CO
O
ty
o
in
o
o
en
t^
in
in
"="
0
u"»
„ ~i
O
rr
en
r*^
en
m
0
o
en
«T
0
-^.
O
C^J
o
o
vO
^
en
—
cn
r^
O
•o-i
O
0
cn
CO
rv.
o
en
in
CM
O
en
o
u-l
O
r^.
—
CM
CM
O
i —
—
CO
o
o
f^.
r^
O
O
__
m
en
^
p^.
CO
f*^.
—
o
r-^
C~*j
cn
o
r-l
«r
CO
o
0
o
o
f^
o
r-^
o
^
'r
o
cn
cn
en
cn
r*^
CO
01
in
O
,_•
r^.
n
r*1
O
cn
r^
r-l
0
en
cn
cn
»— i
CO
CM
CM
""
O
<£-
o
CO
01
o
CO
O")
""
0
0
m
.— .
—
en
0
01
0
o
in
r-i
CO
en
^7-
•^
cn
0
.3
u-l
—1
O
CO
<^-
—
o
o
r^
—m
*y
CO
en
r-
o
o
'^•
f^
in
o
f-^
tM
'—
o
CO
CM
—
01
^~
-~-
c^
o
r-^i
l.-^
CO
—
O"'
—
-
-
j en
i o
in o —
CM ^j CM
< — en — — cn co co o
2: -^.—,-^-_.— o — ^~
t/i ^r |-^ —*• "^ ^^ **™ eo *T"
»J Csj CO ^ ~~ i-rt " £^J f^« r*l
•^ 'in eo f™** ^**j ^^ *^ "^
1^.00500^- — —!
eoeoez-cooeocoeo
r-j
O
3
r-^
O
O
CM
CM
CO
CO
CO
en
o ^~
cn
"V CP
— CM
eo o
co —
en cr.
— — co — '.
— . co en »
-------
co z 31 ~ *o -^ 3131 ••-!
^ < es, —, j-v co ^- — *n
i i C*j o ^ CO CO '.O
Z — CC CO ~ CO *T •T
VI — 31 O -- ~ -~ O
1 .-O u~i — T CD -~i CO
o 31 co 31 3s. co en
z co-- f
V^ i-T> U"i (Nj CD ^J ("""I ^ L^ ^i CN, O1 <—••
U""> ^" CO C^i ^O ^i i^ i^ U~i CO -J~i "v"
t o O — — O
.0000
_J < -"i ^j ^— CD r"i -"> f
-J ^T O CO -^ C^ -"> t
— < x> — 31 :c cn -•i
— i T ^, CO -1 ^Xj (*^
^5 OCO^ICO— ^^, r
" Z. i—' O CO *s. -^ O O
-< '^•'NvC',^w*>~-'^1
i—i <^r_*'~j'^CC'23u~.
S -' j T11 — -1 TT — u^
uo o — ccOLn^c-j
—i cc'^r^o^coao
^ — .n .^, m c^ O
O "^ CO C-. LT1 . — TT '-T. <^ CO
. C1 Cv^ ^^ ^ i — — CO T C j --1
CS '-I O 3". Cj O, — -n 31 •";
31 ^T — • "*. — "•. •— '"i *sr o ^*j ^*i
OOCSOOOOOOOOO
C£ '*~y
< V.
u. i z c- j p- 31 31 co rr si
z< c^rjOTT^r3i
uj ^ u^ ~ T — — CO CO -T. 3-, CO CO
u^ O T C^j -J^ CO u~. ^-« m 31 rx- CO -1
•J1 CO — t
i — un 31
uj^ CITLTIO — rj^j
ca co ^r T f^ T ui o
ci o ^ T en -=r w
ooooooooooo
_i < u-> T co 3s. *^j r" rn
o o o o o o
— z •^•=ro"w^-'=rrr
O — O30 O = >--.
O O i-~. ~» O O CO
O — OOOOOOOr3OO
"^' o — ' — ^>s
O m u^ w-, CO _". r,
O O — ^ ^, «r -.
CT, Z 3"' '-O T fg — CO T
_J < — O -~ O — U-. —
— a-.
, ~* —p _n o — — 31
Z C-, ^i '^ ^ 1^1 C^, ^-* C^i l*^ —~ CO O
v^ ^i *tr jy «o |-O ^. •^ ^3 u™i ™ r^ co
_j m^rrj'^coLr o^oo^o^1"^
o oo — oo o
;o ooo OO
'— -". O —
oooooooooooo
— OCO —
^.Z -- — LT. O
z. < L.-I -v.
< _ O 31 ^ -~:
s_ o ----» — -T ^. u-
CM CO «5- "-, r^ — CO
oz m — ci — co cc =
— < 01 J O -i in _-. —!
_i_ CSl .CO O O CO —1 ~^
— . '-'•3•^. OTtno
-------
-r — o
<--. O
30 O
O O
Ol
-O
a:
Cl.
^- ro —
O O O
O O O
O O O
v^ ~-
O
Z O
O
CM
rn .—i
03
in
— CXI
O
O
o
O
U1
c-.
CO f^J
0 —
C£
=1
O
-------
o
01
2- O O O
o
o
CTl
en
cr>
O CO
CO O~>
O '-o ^ -O
^ r~~ ul — •
CO — f- 'X,
-O ~* T O
51 O SI CD
. — -n o-j co
•a- — O —
O O O O
O O O 3
o o o o
cc
a.
Ol
o
CO
O
— co —
i-- o
en —
UO r-*
CM
CTi
«T CJ1 tO ^*
•"*^ CM CM CM
T LTI O O
r-~ m O CO
co r^ m co
O
Cl
^1 LD
-------
o
r-5
u-.
cn
o o o
o o o
o
U1
o
o
CO
r^
o
CM
co
CO
co rj rn
O CD o
Cl C J Pv.
r*N. u-i —
^ '-O OM,
CD ^-f O
LT"! ^T l^
O O CO en
—• CO f^ f*>
CO CNj — O
0
O
O
000
O O O
O O O
C£.
<
cc
o.
rn
CD
tsj
co
CD
•s:
=3
o-
CO
CO
C-J
CO
o
01
CO r^
CM f—
Oj CM
CO
O
en oj
— CO
o —
T CSI
-------
u~> LD O CO CO CD"rT~*^r^l-riO — "
J ^ O-j
j O O -
^0 cu OG*>CI--•orsj^raaco'^.rx.^-GPii™1 ^
< ^
f— -!T ur» un c\j o CD ca —• o co T u^ —• o f"*. en <>-J'-"
^ ^ CO rn r-
en —J •— •— o o — o
Q
-j C
Q Z Z S£ VI U-i3E2^ZE LU o", V, ;
3: o^juju-iu-izsrzisiZ'-oviLO'-O',
-------
LM Z r»«* O rH <-O CTt C\j
^2: no—"^r^coc^j z<
O^ f^-J CO C\i r
uj UJZ •^'TO'^J'^ CO O
O L/1 <3i —J C1 '"") CO O --* <^r CNj
uj uj __j C\j i»O «•— CT^ C^ cvj CO H~ 2C r*** O^ ^*^ *~* CT^ CO CO C7^ "~" ^O CO 'O
rv. csj O *^ un O C\J O «—• CO CT^ f*)
uj O CO O tJ"1 CTi •-" ^"i u_i Z CO C7> CO O"i C^J n CT^ O O —
r— rx* CD T
O ^^'Ni
CO CTl ^™ ^™ *™^
-------
r-i
O
O1
CO
u CM
o
o
o
ce
O.
<=:
ra
o-
O LT
O cn
O O
o
CO
CO
»M
un
r-^ CM
— CO
a.
Q.
O
O
a:
o
o
— LT>
CO
CM
CO "-
T co
=)
<
O
o.
1^1
a
o
^H —. CM ^~
o o o o
o o n o
o o o o
co
•JS
CO
o
Ol
CSI
o
en
01
CO
CO
0*1
O
CM
O
01
CD
en
m
O
O!
CM
»-|
Oi
us
01
LTI
CO
CM
U-!
^O CO
CM CM
CO CM
f"*i CD Ol
co tn to
ai
CM
CO
CO
CO
— CO
C. —
O ^1
— co
CO
CM
a CM —•
-------
Q
>-
a uj u-i LLJ u-i Z Z Z Z Z 1^1 ul ij-l cy-l^l 3 3 3
-------
C£.
ZD
O
>_uZ CSj — • r-». O •— CO "^
z < ^* r*i *r cri u"i ^~ ^"
i— j -j 'O o*i f~*1 co co r\j co >^j sr ^r ^**. CNJ CD '""i t/^ co n ^*** ^™" *^ co
^C — J v*i C*i «~^ o^ ("^ tn CD r*^ i_i_i ' • ' LO 'Nn CD CD ^
LU O— ' 0"> O j O »—• O^ -^ r
O— J LOO^^tn<^>i-nr^.-— m— «r^.T
"•* ^*^ CO •""
— (-02 ^~
-J < I Z
i— j >• O O
_ I — i «X Z •— ' CNJ m '=T in O r^. CD O\ ^— <
-------
>. . 1.0
LJ O
CD
ro
03
Cf.
Q_
O O O O
O O U"> o
o o — o
"•o ro u") CO
u~>
O
co
CM
r-^
CM
OS
3
O
LJ
O
o
o
o
o
o
o
o
o
o
O
O
<
=>
0-
m
O
i^> —
CM
O
i~-i O
z
i— Z
ca =5
O
CM
CO 0-4 <—
m ^O CTl
vn c>i co
n c^ csj
O *—• f^-
^•^ O^ ^r
CD
rn
o
CO
^J O
CO
O
O
CM
CM
*—• C£
C_ 3
i-J O
O
ce
Cj uj
3- 3
C£ -Z. I
=) i >"
O O <
-------
CO
O
CD
r^
O
0
O
0
O
0
O
o
o
CO U~)
en f--
en en
— CD
— o-.
en co
•— ' LhJ CD
O OO *3"
o s
o
o
CD
o T
— o CM o
m u-» o —'
O
O
o
o
O
CO
o
O£
o-
00
oi
o.
o
o
o
o >a
o —
o o
o
o
o
o
CO
CO
CO
CM CO U1
LT1 CM CM
03
U3
<
Z3
enr
o
*T
CD
o <—
CO
z ~-
3 C-J
u^ CO
tSj CO
Ol CO
fsj r*-.
en —
n ^r
r>. O
o —
CNJ
CO
f*i i—+ CO
O^ CNj Ol
m r*i co
en r>. o
en co —
m m vo
en — o
CSJ U") —.
o
CO
O CNU
o —
o o
<
t—
o
O i—;
>• 3 —
Q£ Z II—
= I >- Z
O C2 < O
n 3 ci s
-------
<=:
u.
3:
CO
en
a:
a.
o
o
o
o
o —
Cxi
= o
o- co
on o
ce.
c_
o
o
o
oo —
CO
O
CSl
un
o
o
en
oo
co
o
en
un
co
CM
m
O
03
o
o
CSl
CSl
un
rn
un
o
a:
O
O
en
Ol
o
oc
o.
o
o
o
o
o
o
o
o
o
o
o
o
o
CNl
Cl
o
o
o
CXl
CO
o
rn
on
z
O on
C3 UJ
ci en
•a: <
LJ =
O O'
c£ un
o
>- 0_
= o
•Z •£.
3 =
O on
z
^
m —
— oo
o
o
o_
>-
en
CSJ
O 00
CO 00
— en
un IT
•-n Oi
o —
rn O
CSJ —.
CSl CSl
O
^r
^i
en
CSJ
CM
un
n
un csj
O Ou
O —
O O
m r^
CSJ r—
<
i—
o
<-j a
C3 on
o
on
-------
CO
03
o
o
o
o
o
o
O
— CO
o «•
<
3
cr
en
en
o
o
— LT)
en ^T
O
o
on
3:
o
o
«T CSJ n-
o co f^
CO — O
O
o
O
CO
t— en
O
CO
ce
a.
o
o
uj O
ee oj
ce
o_
o
O
O
o
o
o
O
CTl
cn
O CM
— O
O
O
O
CO
o
o
o
o
C3- LO
on ~-
CO
CO
Csj
O
co
CO
Ol
en
CT*
CS1
CT>
O
co
o_ ^*
CO — —
vO UO (O
o
-------
—. O •— .-"> en -Xi O O en — cococoocriLnrr —
r-x O C^J U~) O ("^ —
^T C\j — -t —
^ O ^J CD iJ~' O
) r-K CO c*"l O
, CO en CO ^O '•
O CO u~> •—> O^ CC O^,
i—• —> Oj r-v CSj CwOCOCT>O
"^ -O O <-"^ *"n CO
c^ i1*^ co *^ co *^r
^-^Lnr-1^-—
O O"i CTi CO O CTi — " *— ' <^> C^j CO CO CT" ~"
i—OOOOOOO —OO
i~kj ,^ r^ O^j CO O^ ™™
" O (NJ r^*. T— •
CD '•O (*O CD ^^ CO C^
•^ co *T
— • o — *^ o *— • •
I u_i C£ --
2 z z ac ui
-------
O O O u"i '•"I CO — "
o '*•- O *3" i— • TM -sr
O O CO ^ «T ^ CM
r— _o O O «T CM r-v CTi O
O _ I O f! r-^ O fO O O
r— CNj 1— O"> «=•"-"> CM CO
u~J (">- u~> PO CD P"^ CM
LO O r-v O O O ^O
O ^1
i_ < C\j i—« ^* CNj C\J CSJ —^
un z:
_J \^-t "X. C\J C7^ U"> C\J O -^ OO
^*- i^l 2 <£ Cl r^ OD un CO C\i O
I fsj <^ CSj CD LO •-" f^l >- t/1 C?i f^ O O CO rn f*") CSJ ^— O^j CO O
S: U3 CO CTi O O air-- X —I
OGO—OOO X
> — oo — — — <
CM CM LO CO — CM
. rn ui CM UD O r**
t'*^O^''^fN^ CO
li/t un ^" f"O CJ^ ^~" «™^ i^i uw u_i CD u^ O^ *™" ^r CD O^ CD '•O I*O CM CT*
3Z —1 i-O vjO »-^ ^T CD CO CM QD X r*-v CO ^ C**j CO CO CD P-«. CM CM CM ^—
CD ^-Hr\jpn*^LnOr-^
-------
CO
Iff*
o
->
r-i
CSJ
3
CNi -3i
O 3
CSj
ae
O
a.
a
o
a:
O
<
o
ac.
O
QE
a.
uo
1^1
-------
O
in
CM
Oi
Oi
O
O
O
O r*l O
O Ln O
O — O
O —
CM
o-
or
01
o
^- i^j Ol
O
O
o "••")
01 '*•-
n co
f«- CO
*r 01
csj ^~
o —
<•"> O
01
o
o
or
Ol
o
CO
o
Ol
CD
Cr
on
<:
UJ
x
O
o
CO
CM
cn
— UJ
^ o
<-> cr
o — i—
— — Oi
OO t-^
>> u.
= o
—' CM
01 n
O T
•—' in
CO CM
n o
01 co
— 01
o
in
01
co
o
Ol
co
01
r-^
CO
c .n
^- o
c: to
oe >
3 • >-
= 3 rz
-------
o
CD
un
un
C-. — O —
u-> O — O
— O O O
O O O O
ce
Q_
00
CM
CXI
•a-
<:
=>
O-
00
o
on
on
o
CM
CM
O
O
o
t— 00
^D i^
o
0.
on
vO — O —•
O1 O O O
CM O O O
o o o o
o
o
O
O
OD
CD
O
CM
o CM
— us
Co
•o
ai
c
o
o
CO
o
r-1
H5
cn
ro
CO
03
CO
CO
O
00
on
CD m
—. cn
O
I—.
o
cy^ r^
O r-1
•— u~.
CO CM
<*^ CM
CM
*— co
i0 on
cyi cn
O» CO
tn
^~
m
r«N.
LH «T
O^ CSj
-^- —
LT>
— CM
<
O
^ <. ^
-------
LLJ Lf)
Oi
O-
cn
o
o
o
o
o
CD
O
<
=
Cr
o
o
CD
CO
CSI
en
o
o
o
uo O
2: o
I— CM
O CM
O c-l
se csi
tO
o
o
(-1
CSl
ot
=
o
O
as
o.
Q
O
in
m
co
^
CO
o
cc
CL.
O — — —
CO O f) O
l*» O CSJ O
O O n o
CTI
n
CJ
O
u cr
•— on
o
OJ
•£>
in
in
to
O
CTi
— in
L« r~
l~^ CM
^r in
co m
CTi m
O CTi
CTi f^>
i— in
O O
CM
-------
00
C71
cn
r*>
Ol
o
LO
LO
O3
o
o
O
O
o
o
31
CNJ
cn
LO
k-J CM
ce —
•a: CM
= 01
o- o
on ~~
CM ~• — O
— O CD LO
oo
LO
m
O
O
o
CM ~- CO
CM CM CM CM
m f^* ^T Ol
LO <=•
O
O
o
to
o
CM
on
<
on
o
cc
Q.
O
O
s:
o-
on
CM
O
LO
o
in
en
oo
o
CO
o
CTl
CM
O
CM
o —
o o
o o
o
o
o
o
LO
CM
CM
LO
LO
E ce
I- <
O Z3
u- O-
O on
O u.
— O
CO
o
ro
CM
LO
CM
co
en
CM
LO
LO
Ol
LO
o
o
O CO
C1 —
— CM
CM
CO
r^
LO
O
CM
LO
CO
CM
O
LO
co
LO
01
CM
O LO
LO
m
Oi
CM
T
Ol
<
t—
o
Q
O
o ce
ce c:
2: o
o
on
-------
o
o
LT>
01
CD
O O u-> —
O O CO O
o o ~ o
ce
c_
<
rj
o-
CO
cr
Cl
~- *T
i
CXI
i~-
01
U3
o
en
o
o
ce
a.
uj CO
'wO CTt
H- u-i
O ~
O —
ce r«.
o — co o
r-^ —• — Oi
CD in ro o»
CO '^ ^* CO
vD —
CXl r-^
CO
o
m
CM
u-i CO
o
o
o;
a.
^- — CM i—
O O m o
o o — o
o o — o
Cr —
CO
o
CO
CO
<£.
01
o <^i
..— u_j
•a ce
c o-
cu , u-
-= O
en
O
O
CM
CTl f-
CTi
O
CO
co
CM
co
m
LO
^^ LT>
CM
CM
O
CO
«T
CM
CO
u-i u-i
CM en
o o
r— LTl
CM O
r-* CTi
o> 01
CM co
in o
~~ CO
-o
CO
Oi
CM
^~
O1
O
O
ea:
o
ce
3
o
-------
>
(-1
O CTi
o —
o
o
Oi
CS;
cc
CC
CD
CO
CSJ
O
CO
CSl
CS!
o
o —
O T
CO
o
o
in
o
O
O
i/i n
O co
CO 1g*<
CO
— o
T ao
CSj <—
o
Cv
(S)
o
o
CO
01
in
ci
r^
m
co
O
O
ct
a.
— csi <—
O e^ O
O CTi O
o — O
^ O f^ csj
cy^ n ^ 10
01
•a
C£
rs
o-
o
.a
CO
o
co
o
co
csi
co
in
vo
•3-
cr» csj ^r o^
pn ^* ro f*i
*-" CJ\ ^^ CT^
^ co csi r-^
PO CSI P'l f"^
<— Ol T CO
10 in csi r—'
— o
in
o
<~i
CTI
«t
i—
o
o
o
en
=>
o
-------
<
UkJ
X
o
WD
CD
m
03
o
o
o
O
o
o
o
o
LU O
a; —
cz co
= o
Cr r-l
t-n O
CO
CM
o
o
o
in
CO
O co
O —
Qi —
CM
LO
CO in
CM ro
O co
O •—
— C\J —
O O O
O O O
o o o
O
o
o
<
3
O-
CO
CM
O
O
O
O
in
co
O)
o
u u_
— O
CM
in
*T
m
O
m
O
co
CM
—• in
o>
in
in
co
^o
O
O
r**
O
O
oo
O l^i
o
en
i£>
CO
CM
^r
en
o
o
cc
r=
o
k^j * >
-------
>
t_>
; I LD
o
o
o
o
o
o
o
o
co
01
or
Q_
— ffl
CO O
03
CM
O
CM
O
CM
<3" QO CM CM
O
O
o
00 .—'
Z 03
03
i— O
o •=•
O CM
ro i^-s o ^~
r^ o co o
f"^ m co r^v
0*1 ^r in ro
CM
O
LJ
O
c.
oo
O
o
u-l CM »—
n o
r^ O
c~> t—•
ce
o_
o o
o o
o o
CO CM
01 —
o
o
o
o
o
o
CO
id
u_i dj
O F—
CJ
o
en
^T
CM
in
m
O
II
en
O1
co
CM
CM
CO
CM
CM . O —
O CO — O
O ^ ~- r*^
en
o
I t—
3 I >- Z
o a «: o
-------
>
u
o
o
z:
01
or
a.
o
o
o
o
o
o
o
o
or
<
o-
I
sc
O
CO
o
o
o
o
<— t^t
O in
CM O
CM rn
o
CO
m
r^
O1
ro
cn
co
r^
Ol
01
CO
o ui
O "1
or in
O
o.
m
o
o
a:
<:
<£
3
o-
l-hj LH
CO
Cl
u-i
01
r*^
CO
o
^- — O
o o u->
O O O
in •—
CO
o
CM
co
•O'
CM
CO
01
rn
CO
cr.
01
O
CTi
r~-
CTl
co
r^
CTl
O
c^
o
CO
CM
O1
^
n
a>
o
CM
<-> r^
CM —•
<=f
-------
in uj
Csi
O
— — o
ce
o-
O —•
o o
o o
o
o
o
o
O CTi
^ o
OD
CM
on
or
— rv.
O
O
O
O
«T O —
^* co co
CO — CM
o o co
<^n CTi ^-
—• us
o
CM
O
o.
on
Q
O
CO
CO
o
ce
o.
o o o o
o o o o
o o o o
et
UJ
2
O
CM
UJ O
o
U3
CO
CM
O
en
O =>
> O
CM
O
CD
in
O
CO
on
on
— CM
O
10
CO
CO
CO
co
co
•u o
O
CM
CO
— CM
CD —,
O
CO
uj a:
o. =3
uj O
O vO
o
o
OS
o
oc
cc:
=3
o
cc
=>
o
-------
r^. L-J
o s:
CD -J
O O n o
1-1 O o O
CM O CO O
o
CM
CM — —
en
CO
ce
Q.
en
i— o
O to
CD O
a. CM
CM
co
LD
en
oo
CNj
O"l CNj O
CO CO <"*">
CTi fsj —
O^ t-f^ C^
m pv. o
CO CNj C^
o
c_
0-1
o
o
o
o
o
o
en
CM
f^v
CM
O
CO •-" CM
r^ O m
CO O 10
in o co
f-« LT1
en in
O
O
o
OS
O
cz:
<
O
2:
CM
en
en
o
o
CM
en
co
o
GO
en
o
r^ co
co en
o o
CM m
LO ,— i
co
en
co
en
o
o
en —. o
UD CM CM
lO CO
en
o
Oi
=3
o
ac
O
O Q
IT 2
-------
o
CM
o
CO
«: o
z o
CM
_J CO
CM
O
O
O
o
o
C71 CM O CM
•—• O C\j cr
•— CMl O u"~>
<
=)
CD-
a:
a.
O
o
o
o
a:
CO
CM
O
1C
CO
o
en
O
O
co
u->
csj
CNJ
CSJ
O
csj
03
CO
O T
— O
o fn
O OJ
Oi O
^-
-------
Ol
tn
O
o
o
o o*j
O iT>
O Lfl
o
o
<
3
O-
CSj
O
cc
o
— en
CO r^
O
o
o
s o
r"s. <—
•zr r^
(**") ("~i
P-. m
co <^i
r^i ^T
O —
CO
o
O
10
a.
a.
o
o
CC
CTV
O
O
Q.
a
o
o- —
00 CO
CO
Z r>»
<
uj O
01
co
o
CTi
ct:
a.
in
O
O
co
o
— o —
o in o
o ai o
o ro o
< cc:
s <
O iyi
a:
O u.
—i O
us —
csj
CT>
o
CTl
t\j
en
^D 1^1 ^"
LO CM O
^^ i-n co r**.
c\j ^r ro ^D
LO •—' r^s. rv.
O CO CT> O
n «T o o
^j o:
c_ =
i_j O
o
e::
-------
cc
01
o o
— o o
01 o o
o
o
o
o
o
<
LU
Z
o
Cl
un
CM
CM
10
CO
*r
o
un
Oi
co
o
o
cr
u-l
03
o
00
un
r^ *-•
uO O
CM
un
m
o
ae
o
!
O
cc:
o
^^ m
Ci
-O
m
uo
co ao
o cn
CM
CO
o
o
u.
OL
CO
= i
O O
-------
ce
CL.
o
O
o —
o o
o
CO
Ol
in
CM
m
— CM
in o
•a- —
O
o
o;
CO
LD
CTl
01
^o
CM
oc
3
Q
IX
a.
LD *— LT) —'
^ O tr> O
r^l O eg O
O O — O
O1
<-">
>£>
uo
O
CO
O
Oi
CO
— ^- o
o —
a:
o
-~ CT\ CM
O m CD
^O O
l£> CNj
lO CO
in o
CNJ
CM
m
Ol
CM
CO
co
CT1 rn
u^ in
in —
o
CM
— c in
I
o
-------
CD
C1
CM
CD
cr
CM
CO
01 Cn
o —
o
o
<:
CO-
CM
CM
CO
CO
o
o
C£
Q.
o
o
CM
CO
u-i
CO
ci
en
o
O
ce
O
f-J
o
CO
CO
CO
en
en
o
G-
uo
o
o
co — •
i~-» en
en T ui
u-i o —
en
co
o
o
en
o
•r
O
CM
ee
o.
O
cn
o — < ^~
cc: u-<
O OL
-------
O
O
ex
O
O
O
o
o
CM i~ O
o- —
i^l O
-n CM
<=• CD
CD —
^O Ol
m o
CM —
CM —
o
o
O
CD
CM
O
O
O
O
O
^* LO
O
as
Q-
ce
<£
CM
en
O
co
o
O
to
o
co
m
in
in
o
o
oc
a.
— CD — —•
r~ — O O
cvj on O O
O O O O
,-. O —
co
Oi
oo
CM
o
O
co
r~. O
O ~-
O1
cn
01
o
CM
co
CM
CO
O
o
m
01
co
CM
10
O1
O
«
u_
O
c_ 3
Q
O
a;
o
Ci
O
^:
^> i^j
O 2
I >-
O <
-------
in
in
O
O
•3-
<*>
O
cc
o_
O
o
o o
O •=!
o
o
03
CsJ
LT,
or
CO
O
(J-l
1/1
— co
CO Ol
— 01
oe
O-
o
o
o
CD
VO
CO
•3- CD
CO —
O
O
o
0.
on
a:
<
3
cn
03
in
CM
O
CO
in
O
1/1
O
03
o
QC
CL.
O
O
O
o
o
o
o
o
o
o
o
UJ f O
TI in in in
CM CO ""^ C31
f^ ^- rn CO
CM
en o
co co
O en
co CP
m
m
O O
or
o z
o
co
01
in
CM
O
CM
CO
CD
CO C1
CM
3 i
o a
-------
LJ
o
o
CO
C£.
Q_
o
o
o
o
CO
o
31
CO
< CM
= CO
o- —
on o
O
o
a;
a.
O
O
cr:
^ co in ^c
en — T en
in —
CO
o
C£
O_
u^ in
o
en
CM
O
z z
3 3
O t/l
CM
VO
O
•3-
CO
O
O
o
o
co
CM
CO
CM
O
CM
f^
T
CM
CO
en
o
o
co
CM
co
co
crv
CM
o
en
o
m
en
CM
^~
en
o
o
— o o
o
a;
<: o
=. z
-------
_j <:
CO CM CO CM — • en cc en —
cc o O T co — ' CD ^- cc O i-r; --, o
CM CM C\j (**"> CM •— a") en CO C1 "^ -"> r-- LH Cn 32 ^ -" r~ rr _-,
CM Cn *^T ~*- ^~
^TLDOLO'C'^Tr^u-iuncorn — • O — - ^•
en — CM:DfMP--CnO'-*-CMCO'-"i'— •r-^Ln
cn r^ r>. en cn P*- ^^ r-1- u"l U"> CD uO O CM —
«— « PH CM O <""> r"1 CO «— CO Cn Cn Cn csj r^.^
OOOOOOOOOOOOOOGCDO;; o —
-oo -
^^ *^ i-O O LHO'
I/-) r—* l*~.
_l CO —
i ^^ •"" ^J ^' CO tO «-^ CO *
*"• CO CNj -^~) CO 'O
__j ^^ i"f** p—* c\j ^r ^>
LJ ^ <""") *C" T —"'^OCDO1^'-
1 CO " r"> 1^1 CO O CO G" '" J " - CO •-
CO -* — O "-J —
O.
1/1
o
2:
CO CT> CD CO O^ CO O"l -O 'Vfc C7i ^T C\j t™™ C7^ f^** ^^ CO CO >«O f^1* ^*« *
CO CO CD CO CO CO CO CO CO CO CTv O '—' C\j r^. CO O"> CTi CTi CO CO CO CO CO
^ CO
^-« i^ >o ^ Csj CD i"*"l *"— ^^ -fl O^ d ^- C*' ^
CNJ C\J CN4 CSJ —* Cv. O — O """I "~ C\J — -— ^ -^
ooooooooooooo
< VI
Z I—
— VI
000
} Cs* CTi CO i^1 — • r
. tri O O O CO ^-s •— * Cfi •— r
— . ^— — (Ng ^^
CTif*x-^"rili^O CO i-H CD C?^ CT1 '-^ CO (*") CO
—^ CNj O^ Cfi •"" CSJ CO O <*") -~ '^ ^^ O ^-J
Oj CO (^i O — « O ^*
*—• CSJ C\J CNj C\J CSJ CSJ C\| CSJ CM
"CO O CO CO — CO
en en en en en en co en en en en "•" co >^ co en co co co en en o*> o*> en
Cn.OO en "-• en in ^. i*^ \o <^ ^— o f*-* CM r^. — co ^"
- *~* O P*-. p*"- ^" u*> ^" rn r^i u^ f^i o ^ O <-n en
'~ Lf"' '~- O r--. '^- r^i r^ r-*, — .;o
ocoocoocoocooooo — cocooocreo
("> ^— Csj ^ *^ ^0 i o -^^ CO xT^ O> •
O O — f -J '
^ O — CM r- •*? •."> o -~ co cn .— — — -
-------
< in CM LO
J u-i CM T" un
IZ i-~ CO O
I V> ^- !—)CM
—J G COCM
1-1 CM -—!
^r O-' O
cr> co
z: z en —o
<
•z.
IS1
CV "xa r-l o
LO O O —
O — f": f>
O
3D
LJ
O o-i
C5 C£
z <
cs cr
< 1/5
U«i
Z I—
at < — OCM
u- s comco
ce iyi UDOO
Z z en co in
UJ UkJ CM "T* CO
-j on n m m
t_i _i o «• f*i
O OOO
OOO
CM
"3"
CO
r"i
CSJ
O
cr\
CO
in
O"l CM
o —
o
co
en
co
CD
CO
o
o
CO
CO
CO
CM
rsj
«T
C-J
U1
CO
•3 — O
^r oo r*^
-o en ~-
cn co en
o o CM
— o — o —
o
o
«x in o CM
T m
CM ^*
— O
o
o
en
co
co
—) ^£ en en 10
LJ c: m c\
L^J tn —' <
— como
> in co o
in
o —
— — LO •—i — — 'CMCMCMCM
-------
TECHNICAL REPORT DATA
/Phase r<_~d Ins;ruc;ioi:s (..n the rc:ers< Ui fort- co
i REPORT NO
EPA-45Q/4-88-QD7
|3 RECIPIENT'S ACCESS'ON NC
I
4 TITLE AND SUBTITLE
Statistical Properties of Hourly Concentrations of
Volatile Organic Compounds At Baton Rouge, Louisiana
6 PERFORMING ORGAN!ZAT ON CODS
5 REPOR" DATE
May 1938
7 AUTHOR(S)
Alison K. Pollack, Thomas J. Permutt and Mithra Moezzi
a. PERFORMING ORGANIZATION
9 PERFORMING ORGANIZATION NAME AND ADDRESS
Systems Applications, Incorporated
101 Lucas Valley Road
San Rafael, California 94903
10 PROGRAM ELEMENT NO
11 CONTRACT GRANT ^
68-02-4331
12 SPONSORING AGENCY NAME AND ADDRESS
Monitoring and Reports Branch (MD-14)
U.S. Environmental Protection Agency
Research Triangle Park, NC 27711
13. TYPE OF REPORT AND PERIOD CO v£ = E;
14 SPONSORING AGENCv COCH
15 SUPPLEMENTARY NOTES
EPA Project Officers: William F. Hunt, Jr., and Robert B. Faoro
16 ABSTRACT
Hourly measurements of 16 volatile organic compounds (VOC) in downtown Baton
Rouge, Louisiana have been monitored since 1984. These are probably the most
extensive data of hourly air toxics concentrations in the United States collected to
date. In this report, we discuss the results of an exploratory data analysis of
nearly two years of hourly concentrations. Although we analyzed the data, the
discussion centers on benzene, a known human carcinogen.
17
a
Statistical
VOC
Benzene
Carcinogen
Baton Rouge
18 DISTPI8UTIOI1
Unl i mi ted
EPA Form 2220-1
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
Properties
Hourly Monitoring
Toxics
Data Analysis
~t STATEMENT
b IDENTIFIERS/OPEN ENDED TERMS
19 SECURITY CLASS /This Report'
20 SECURITY CLASS i This page,
t. COSATI 1 iclj Group
21 NO OF °AG£S
204
22 PRiCE
(Rev 4-77) PREVIOUS £ = IT
------- |